Flame-retardant resin composition

ABSTRACT

A flame-retardant resin composition comprises a base resin (e.g., a polyester-series resin), a flame retardant (A) comprising a salt of an amino group-containing triazine compound with a sulfuric acid and/or a sulfonic acid, a flame-retardant auxiliary (B). The flame-retardant auxiliary (B) includes an aromatic resin, acyclic urea-series compound or a derivative thereof [e.g., acetyleneurea, uric acid, a salt of melamine or a condensate thereof (e.g., melam, melem, and melon) with cyanuric acid], an amino group-containing triazine compound (e.g., melamine or a condensate thereof), and/or an inorganic metal-series compound (e.g., a metal salt of an oxygen acid having no sulfur atom, a metal oxide, a metal hydroxide, and a metal sulfide). The present invention provides a flame-retardant resin composition to which flame retardancy is imparted without using a halogen-series flame retardant and an organic phosphorus-series flame retardant.

This application is the US national phase of international applicationPCT/JP20041007101 filed 25 May 2004 which designated the U.S. and claimsbenefit of JP 2003-148215, dated 26 May 2003, the entire content ofwhich is hereby incorporated by reference.

TECHNICAL FIELD

The present invention relates to a flame-retardant resin compositionuseful for flame retardation of a thermoplastic resin such as apolyester-series resin, and a process for producing the same, and ashaped article formed from the flame-retardant resin composition.

BACKGROUND ART

A thermoplastic resin, for example a polyester-series resin, hasexcellent mechanical and electrical properties, weather resistance,water resistance, and resistance to chemicals and solvents. Therefore,the resin is used as an engineering plastic in various purposes such aselectric or electronic device parts, mechanical device parts andautomotive parts. While, the polyester-series resin is required to haveimproved mechanical properties and to be flame-retardant from viewpointof safety as the field of their uses expands. As a flame retardant forgenerally imparting high flame-retardancy to a resin, a halogen compoundor an organic phosphorus-containing compound has been known. However, ahalogen-containing flame retardant is not preferable for environmentalreasons because the flame retardant sometimes generates a large amountof a dioxin-series compound on resolution caused by combustion. Inaddition, an organic phosphorus-containing flame retardant is acausative factor of a sick house syndrome which has been a problemrecently, and is not preferred from the viewpoint of safety.

On the other hand, there has been proposed a flame-retardant resincomposition to which flame retardancy is imparted by using a flameretardant which is not an organic phosphorus-containing nor halogenatom-containing one. For example, Japanese Patent Application Laid-OpenNo. 255811/1997 (JP-9-255811A) (Patent Document 1) discloses aflame-retardant resin composition which comprises a thermoplastic resinsuch as a polystyrene resin, a polypropylene resin or a polyamide resin,and a reaction product of melamine and sulfuric acid as a flameretardant. Moreover, Japanese Patent Application Laid-Open No.511409/1998 (JP-10-511409A) (Patent Document 2) discloses that amelamine condensate which is obtained from condensation of melamine or amelamine salt by using an organic acid such as sulfonic acid impartsflame retardancy to a polyamide resin, an ABS resin, and a polyurethaneresin. Further, Japanese Patent Application Laid-Open No. 288361/2001(JP-2001-288361A) (Patent Document 3) discloses a flame-retardantpolyamide resin composition containing melam methanesulfonate as a flameretardant.

These flame retardants, however, cannot certainly impart enough flameretardancy to a broad variety of resins (in particular, apolyester-series resin).

Patent Document 1: JP-9-255811A

Patent Document 2: JP-10-511409A

Patent Document 3: JP-2001-288361A

DISCLOSURE OF THE INVENTION Problems to be Solved by the Invention

It is therefore an object of the present invention to provide a resincomposition which is rendered flame-retardant to a satisfactory levelwithout using a halogen-containing flame retardant and/or an organicphosphorus-containing flame retardant, a process for producing the same.

Another object of the present invention is to provide a flame-retardantresin composition of high practical use without deterioratingcharacteristics of a base resin, a process for producing the same.

It is still another object of the present invention to provide a shapedarticle which improves flame retardancy and inhibits bleeding out, and aprocess for producing the same.

It is a further object of the present invention to provide a shapedarticle which is improved in both flame retardancy and electricalproperties (e.g., tracking resistance), and a process for producing thesame.

Means to Solve the Problems

The inventors of the present invention made intensive studies to achievethe above objects and finally found that the combination use of aspecific flame-retardant auxiliary and a salt of an aminogroup-containing triazine compound with a sulfuric acid and/or asulfonic acid imparts flame retardancy to a base resin (e.g., athermoplastic resin) at a high level without using a halogenatom-containing or a phosphorus atom-containing flame retardant. Thepresent invention was accomplished based on the above findings.

That is, the flame-retardant resin composition of the present inventioncomprises (R) a base resin, (A) a flame retardant and (B) aflame-retardant auxiliary, wherein the flame retardant (A) comprises asalt of (Al) an amino group-containing triazine compound [for example,melamine and a melamine condensate (e.g., melam, melem, and melon)] with(A2) at least one member selected from the group consisting of asulfuric acid and a sulfonic acid (for example, an alkanesulfonic acid),and the flame-retardant auxiliary (B) comprises at least one memberselected from the group consisting of (B1) an aromatic resin, (B2)acyclic urea-series compound or a derivative thereof, (B3) an aminogroup-containing triazine compound and (B4) an inorganic metal-seriescompound.

The base resin (R) may comprise at least a polyester-series resin. Thebase resin (R) may comprise (i) a polyester-series resin (for example,an aromatic polyester-series resin such as a homo- or copolyester havingat least one unit selected from the group consisting of1,4-cyclohexanedimethylene terephthalate, a C₂₋₄alkylene terephthalate,and a C₂₋₄alkylene naphthalate, or the like), or (ii) thepolyester-series resin and a polystyrenic resin. The base resin (R) maybe, for example, a polyC₂₋₄alkylene terephthalate (e.g., a polyethyleneterephthalate (PET), a polypropylene terephthalate [(PPT), apolytrimethylene terephthalate (PTT)], and a polybutylene terephthalate(PBT)), or a modified polyC₂₋₄alkylene terephthalate (e.g., anisophthalic acid-modified polybutylene terephthalate), and others.Moreover, the base resin (R) may be a mixture of a plurality ofC₂₋₄alkylene terephthalates, for example, a mixture of a first resin anda second resin, wherein the first resin is a polyC₃₋₄alkyleneterephthalate (PPT, PBT), and the second resin is PET or PBT and is fromthe first resin. Such a mixture may include, for example, (i) a mixtureof PBT and PET, (ii) a mixture of PPT and PET, (iii) a mixture of PPTand PBT, and others. The proportion of the first resin relative to thesecond resin [the first resin/the second resin] may be 20/80 to 80/20(e.g., 30/70 to 80/20) in a weight ratio.

The proportion of the amino group-containing triazine compound (A1)relative to the total amount of the sulfuric acid and the sulfonic acid(A2) [the component (A1)/the component (A2)] is about 1/5 to 5/1 in amolar ratio. Moreover, the salt of the amino group-containing triazinecompound with the sulfuric acid and/or the sulfonic acid may have aweight decrease of not larger than 15% by weight (e.g., about 0.001 to15% by weight) when the salt is heated with increasing a temperaturefrom 30 to 250° C. at an increasing rate of 20° C. per minute under anitrogen flow.

In the flame-retardant auxiliary (B), the aromatic resin (B1) maycomprise an aromatic ring having a hydroxyl group and/or an amino group,a polyarylate-series resin, an aromatic epoxy resin, an aromatic nylon,a polyphenylene sulfide-series resin, a polyphenylene oxide-seriesresin, a polycarbonate-series resin, and others. The cyclic urea-seriescompound or a derivative thereof (B2) may comprise a cyclic ureide [forexample, a cyclic monoureide (e.g., cyanuric acid, and isocyanuricacid), and a cyclic diureide (e.g., acetyleneurea, and uric acid)], anda salt of the cyclic ureide with a melamine (e.g., melamine, melam,melem, and melon). The amino group-containing triazine compound (B3) maybe melamine or a derivative thereof (e.g., melamine or a melaminecondensate), guanamine or a derivative thereof [for example, guanamine,benzoguanamine, phthaloguanamine, adipoguanamine, CTU-guanamine, aguanamine compound having a heterocycle-containing group as asubstituent (e.g., 2,4-diamino-6-(2′-imidazolyl-(1′)-alkyl)-s-triazine)which may have an alkyl group and/or an aryl group at a ternary carbonatom of an imidazole ring thereof], and others. The inorganicmetal-series compound (B4) may be a metal salt of an inorganic acid [forexample, a metal salt of an oxygen acid having no sulfur atom (e.g., ametal borate, a metal hydrogen phosphate, and a metal stannate)], ametal oxide, a metal hydroxide, a metal sulfide, and others.

In the flame-retardant resin composition, for example, the base resin(R) may comprise at least a polyester-series resin, the flame retardant(A) may comprise a salt of at least one aminotriazine compound selectedfrom the group consisting of melamine and a condensate thereof with atleast one member selected from the group consisting of the sulfuric acidand the sulfonic acid (e.g., an alkanesulfonic acid such asmethanesulfonic acid), and the flame-retardant auxiliary (B) maycomprise the aromatic resin (B1) (e.g., an aromatic epoxy resin).Moreover, in the flame-retardant resin composition, for example, thebase resin (R) may comprise at least an aromatic polyester-series resin,the flame retardant (A)may comprise a salt of at least one aminogroup-containing triazine compound selected from the group consisting ofmelamine and a condensate thereof with at least one member selected fromthe group consisting of the sulfuric acid and a sulfonic acid, and theflame-retardant auxiliary (B) may comprise at least one member selectedfrom the group consisting of acetyleneurea, uric acid, a salt ofmelamine or a condensate thereof with cyanuric acid, and melamine or acondensate thereof. Incidentally, in the flame retardant (A) and theflame-retardant auxiliary (B), the melamine condensate may be at leastone member selected from the group consisting of melam, melem, andmelon.

In the flame-retardant resin composition, the proportion of the flameretardant (A) relative to the flame-retardant auxiliary (B) [the flameretardant (A)/the flame-retardant auxiliary (B)] may be about 99.99/0.01to 1/99 in a weight ratio. Incidentally, the proportion of the flameretardant (A) relative to the aromatic resin (B1) may be about99.99/0.01 to 20/80 in a weight ratio. The flame-retardant resincomposition may contain 10 to 120 parts by weight of the flame retardant(A) and 0.001 to 5 parts by weight of the flame-retardant auxiliary (B)relative to 100 parts by weight of the base resin (R).

The flame-retardant resin composition of the present invention mayfurther comprise at least one member selected from the group consistingof an antioxidant, a stabilizer, a dripping inhibitor, a lubricant, aplasticizer and a filler.

Moreover, the present invention includes a process for producing aflame-retardant resin composition, which comprises mixing (R) a baseresin, (A) a flame retardant, and (B) a flame-retardant auxiliary, andalso includes a shaped article formed from the above-mentionedflame-retardant resin composition.

The shaped article may have, as an electrical property, a comparativetracking index of not less than 300 V (e.g., not less than 350 V), andhave, as a flame retardancy, a flame-retardant performance of V-2, V-1or V-0 in a flame retardancy test measured by using a test piece havinga thickness of 0.8 mm in accordance with UL94. The shaped article may bean electric and/or electronic device part, an office automation devicepart, an automotive part, or a mechanical part or machine element.Moreover, the shaped article may be a connector part, a switch part, arelay part, a transformer part, a breaker part, an electromagneticswitch device part, a focus case part, a capacitor part, a motor part, acopying machine part, or a printer part.

The present invention further includes a process for producing a shapedarticle, which comprises injection-molding a flame-retardant resincomposition containing (R) a base resin, the flame retardant (A) and (B)the flame-retardant auxiliary.

EFFECTS OF THE INVENTION

According to the present invention, combination use of (A) a salt of anamino group-containing triazine compound with a sulfuric acid and/or asulfonic acid and (B) a specific flame-retardant auxiliary imparts flameretardancy to a base resin at a high level without using ahalogen-containing flame retardant and/or an organicphosphorus-containing flame retardant even when the proportion of theflame retardant is low. Moreover, according to the present invention,flame retardancy can be imparted to the base resin without deterioratingcharacteristics of the base resin, and a resin composition of muchpractical use can be obtained. Further, the present invention ensuresboth improvement in flame retardancy and inhibition of bleeding out of ashaped article. Furthermore, according to the present invention,electrical properties (e.g., tracking resistance) of the shaped articlecan be also improved.

DETAILED DESCRIPTION OF THE INVENTION

[Base Resin]

The base resin (R) includes various thermoplastic resins utilizable formolding process, and for example, a polyester-series resin, a styrenicresin, a polyamide-series resin, a polycarbonate-series resin, apolyphenylene oxide-series resin, a vinyl-series resin, an olefinicresin, an acrylic resin, and others. These base resins may be usedsingly or in combination.

(1) Polyester-Series Resin

The polyester-series resin is a homopolyester or copolyester obtainedby, for example, a polycondensation of a dicarboxylic acid component anda diol component, a polycondensation of a hydroxycarboxylic acid or alactone, or a polycondensation of these components. The preferredpolyester-series resin usually includes a saturated polyester-seriesresin, in particular an aromatic saturated polyester-series resin.

The dicarboxylic acid component may include, for example, an aliphaticdicarboxylic acid (e.g., a dicarboxylic acid having about 4 to 40 carbonatoms such as succinic acid, adipic acid, suberic acid, sebacic acid,dodecanedicarboxylic acid or dimeric acid, preferably a dicarboxylicacid having about 4 to 14 carbon atoms), an alicyclic dicarboxylic acid(e.g., a dicarboxylic acid having about 8 to 12 carbon atoms such ashexahydrophthalic acid), an aromatic dicarboxylic acid [for example, adicarboxylic acid having about 8 to 16 carbon atoms, e.g., anarenedicarboxylic acid (e.g., phthalic acid, isophthalic acid,terephthalic acid, and a naphthalenedicarboxylic acid such as2,6-naphthalenedicarboxylic acid), a bisphenyl-dicarboxylic acid (e.g.,4,4′-biphenyldicarboxylic acid, diphenylether-4,4′-dicarboxylic acid, adiphenylalkanedicarboxylic acid (e.g., 4,4′-diphenylethanedicarboxylicacid), and diphenylketonedicarboxylic acid], or a derivative thereof(e.g., a derivative, capable of producing an ester, such as a loweralkyl ester, an aryl ester, and an acid anhydride). These dicarboxylicacid components may be used singly or in combination. Further, ifnecessary, the dicarboxylic acid component may be used in combinationwith a polycarboxylic acid such as trimellitic acid or pyromelliticacid.

The preferred dicarboxylic acid component includes an aromaticdicarboxylic acid such as terephthalic acid, isophthalic acid, ornaphthalenedicarboxylic acid.

As the diol component, for example, there are mentioned an aliphaticalkylene glycol (e.g., an aliphatic glycol having about 2 to 12 carbonatoms such as ethylene glycol, trimethylene glycol, propylene glycol,1,4-butanediol, neopentyl glycol or hexanediol, preferably an aliphaticglycol having about 2 to 10 carbon atoms), a polyoxyalkylene glycol[e.g., a glycol having a plurality of oxyalkylene units of which thealkylene group has about 2 to 4 carbon atoms, for example, diethyleneglycol, dipropylene glycol, ditetramethylene glycol, triethylene glycol,tripropylene glycol, and a polytetramethylene glycol], an alicyclic diol(e.g., 1,4-cyclohexanediol, 1,4-cyclohexanedimethanol, and hydrogenatedbisphenol A), and others. Moreover, the diol component may be used incombination with an aromatic diol such as hydroquinone, resorcinol,biphenol, 2,2-bis(4-hydroxyphenyl)propane,2,2-bis-(4-(2-hydroxyethoxy)phenyl)propane, or xylylene glycol. Thesediol components may be used singly or in combination. Further, ifnecessary, the diol component may be used in combination with a polyolsuch as glycerin, trimethylolpropane, or pentaerythritol.

The preferred diol component includes a C₂₋₆alkylene glycol (e.g., alinear alkylene glycol such as ethylene glycol, trimethylene glycol,propylene glycol or 1,4-butanediol), a (poly)oxyalkylene glycol having arepeating oxyalkylene unit of about 2 to 4 [a glycol containing a(poly)(oxy-C₂₋₄alkylene) unit, such as diethylene glycol], and1,4-cyclohexanedimethanol.

The hydroxycarboxylic acid may include, for example, a hydroxycarboxylicacid such as hydroxybenzoic acid, hydroxynaphthoic acid, glycolic acidor lactic acid, or a derivative thereof.

Examples of the lactone may include a C₃₋₁₂lactone such as propiolactoneor caprolactone (e.g., ε-caprolactone), and others.

The preferred polyester-series resin includes a homopolyester orcopolyester containing an alkylene arylate unit such as an alkyleneterephthalate or an alkylene naphthalate as a main unit (e.g., about 50to 100% by weight, preferably about 75 to 100% by weight) [for example,a homopolyester such as a polyalkylene terephthalate (e.g., apolyC₂₋₄alkylene terephthalate such as a poly(1,4-cyclohexanedimethyleneterephthalate) (PCT), a polyethylene terephthalate (PET), apolypropylene terephthalate (PPT) [PPT (a homopolyester obtained bypolycondensation of a terephthalic acid component and a propylene glycolcomponent), a polytrimethylene terephthalate (PTT) (a homopolyesterobtained by polycondensation of a terephthalic acid component and atrimethylene glycol component)], or a polybutylene terephthalate (PBT)),a polyalkylene naphthalate (e.g., a polyC₂₋₄alkylene naphthalate such asa polyethylene naphthalate, a polypropylene naphthalate or apolybutylene naphthalate); and a copolyester containing alkyleneterephthalate and/or alkylene naphthalate unit(s) as a main unit(e.g.,not less than 50% by weight)]. The particularly preferredpolyester-series resin includes a polybutylene terephthalate-seriesresin containing a butylene terephthalate unit as a main unit [e.g., apolybutylene terephthalate, and a polybutylene terephthalate copolyester(for example, a comonomer-modified PBT, e.g., a PBT modified (orcopolymerized) with an asymmetric dicarboxylic acid, such as isophthalicacid-modified PBT (or isophthalic acid-copolymerized PBT))], apolyethylene terephthalate-series resin containing an ethyleneterephthalate unit as a main unit (e.g., a polyethylene terephthalate,and a polyethylene terephthalate copolyester), and apolypropylene-series resin (e.g., a polypropylene terephthalate, and apolypropylene terephthalate copolyester). Incidentally, thesepolyester-series resins may be used singly or in combination.

Moreover, in the copolyester, a copolymerizable monomer (a comonomer)may include a C₂₋₆alkylene glycol (e.g., a linear or branched alkyleneglycol such as ethylene glycol, propylene glycol or 1,4-butanediol), a(poly)oxyalkylene glycol which has a repeating oxyalkylene unit of about2 to 4 (e.g., a glycol containing a (poly) (oxy-C₂₋₄alkylene) unit, suchas diethylene glycol), a C₆₋₁₂aliphatic dicarboxylic acid (e.g., adipicacid, pimelic acid, suberic acid, azelaic acid, and sebacic acid), anaromatic dicarboxylic acid (e.g., phthalic acid, isophthalic acid, anddiphenyldicarboxylic acid (in particular, an asymmetric aromaticdicarboxylic acid such as phthalic acid or isophthalic acid)), ahydroxycarboxylic acid (e.g., hydroxybenzoic acid, and hydroxynaphthoicacid), a salt of sulfo-aromatic dicarboxylic acid [for example, analkali metal salt of sulfoisophthalic acid (e.g., 5-sodiumsulfoisophthalate), and a phosphonium salt of sulfoisophthalic acid].Incidentally, the polyester-series resin may have not only a linearchain structure but also a branched chain structure, or crosslinkedstructure as far as melt-moldability thereof is not deteriorated.Moreover, the polyester-series resin may be a liquid crystallinepolyester.

The polyester-series resin may be a mixture of a plurality of resinsdifferent in the species (e.g., a C₂₋₄alkylene glycol). Such a mixturemay include a mixture of a first resin selected from C₃₋₄alkyleneterephthalates (PPT, and PBT) and a second resin (e.g., a polyethyleneterephthalate or a polybutylene terephthalate) different from the firstresin, for example, (i) a mixture of a polybutylene terephthalate and apolyethylene terephthalate, (ii) a mixture of a polypropyleneterephthalate and a polyethylene terephthalate, and (iii) a mixture of apolypropylene terephthalate and a polybutylene terephthalate. Amongthese mixtures, a mixture of a polybutylene terephthalate and apolyethylene terephthalate, or a mixture of a polypropyleneterephthalate and a polyethylene terephthalate is particularlypreferred.

In the resin mixture, the proportion of each resin is not particularlylimited to specific one, and for example, the proportion (weight ratio)of the first resin relative to the second resin [the first resin/thesecond resin] may be about 20/80 to 80/20, preferably about 30/70 to80/20 (e.g., about 30/70 to 75/25), and more preferably about 35/65 to70/30.

The polyester-series resin may be produced by a conventional manner, forexample, transesterification, direct esterification.

(2) Styrenic Resin

As the styrenic resin, for example, there may be mentioned a homo- orcopolymer of a styrenic monomer (e.g., styrene, vinyltoluene, andα-methylstyrene); a copolymer of the styrenic monomer and a vinylmonomer [e.g., an unsaturated nitrile (such as acrylonitrile), anα,β-monoolefinic unsaturated carboxylic acid or an acid anhydridethereof or an ester thereof (such as a (meth)acrylic acid ester,(meth)acrylic acid or maleic anhydride)]; a styrenic graft copolymer;and a styrenic block copolymer.

The styrenic resin may include a polystyrene [GPPS, and SPS (asyndiotactic polystyrene)], a styrene-methyl methacrylate copolymer, astyrene-(meth)acrylic acid copolymer, a styrene-acrylonitrile copolymer(AS resin), a graft copolymer in which a styrenic monomer and, ifnecessary, a copolymerizable monomer (at least one member selected fromthe group consisting of acrylonitrile and methyl methacrylate) isgraft-polymerized to a rubber component (e.g., a polybutadiene, anacrylic rubber, and a styrene-butadiene copolymer rubber) [for example,a high impact polystyrene (HIPS), an ABS resin, and an MBS resin], ablock copolymer comprising a polystyrene block and a diene or olefinblock [for example, a styrene-butadiene-styrene (SBS) block copolymer, astyrene-isoprene block copolymer, a styrene-isoprene-styrene (SIS) blockcopolymer, a hydrogenated styrene-butadiene-styrene (SEBS) blockcopolymer, and a hydrogenated styrene-isoprene-styrene (SEPS) blockcopolymer, an epoxidized SBS, and an epoxidized SIS]. These styrenicresins may be used singly or in combination.

(3) Polyamide-Series Resin

The polyamide may include a polyamide derived from a diamine and adicarboxylic acid; a polyamide obtained from an aminocarboxylic acid,and if necessary in combination with a diamine and/or a dicarboxylicacid; a polyamide derived from a lactam, and if necessary in combinationwith a diamine and/or a dicarboxylic acid. The polyamide may alsoinclude a copolyamide. Each of the diamine, the dicarboxylic acid, theaminocarboxylic acid, and the lactam may be used singly or incombination.

As the diamine, there may be mentioned, for example, a C₃₋₁₀aliphaticdiamine such as tetramethylenediamine or hexamethylenediamine, and analicyclic diamine such as bis(4-aminocyclohexyl)methane orbis(4-amino-3-methylcyclohexyl)methane. If necessary, the diamine may beused in combination with an aromatic diamine such as phenylenediamine ormetaxylylenediamine.

Examples of the dicarboxylic acid may include a C₄₋₂₀aliphaticdicarboxylic acid such as adipic acid, suberic acid, sebacic acid ordodecanoic diacid; a dimerized fatty acid (dimeric acid); an alicyclicdicarboxylic acid such as cyclohexane-1,4-dicarboxylic acid orcyclohexane-1,3-dicarboxylic acid; an aromatic dicarboxylic acid such asphthalic acid, phthalic anhydride, isophthalic acid, terephthalic acidor naphthalenedicarboxylic acid; and others.

As the aminocarboxylic acid, there may be mentioned, for example, aC₄₋₂₀aminocarboxylic acid such as aminoheptanoic acid, aminononanoicacid or aminoundecanoic acid. As the lactam, for example, there may bementioned a C₄₋₂₀lactam such as caprolactam or dodecalactam.

The polyamide-series resin may include an aliphatic polyamide (such as anylon 46, a nylon 6, a nylon 66, a nylon 610, a nylon 612, a nylon 11 ora nylon 12), a polyamide obtainable from an aromatic dicarboxylic acid(e.g., terephthalic acid and/or isophthalic acid) and an aliphaticdiamine (e.g., hexamethylenediamine, and nonamethylenediamine), apolyamide obtainable from both aromatic and aliphatic dicarboxylic acids(e.g., both terephthalic acid and adipic acid) and an aliphatic diamine(e.g., hexamethylenediamine), and others. These polyamide-series resinsmay be used singly or in combination.

(4) Polycarbonate-Series Resin

The polycarbonate-series resin may include a polymer obtainable throughthe reaction of a dihydroxy compound (e.g., an alicyclic diol, and abisphenol compound) with phosgene or a carbonic ester such as diphenylcarbonate. Examples of the bisphenol compound may include abis(hydroxyaryl)C₁₋₁₀alkane such as bis(4-hydroxyphenyl)methane or2,2-bis(4-hydroxyphenyl)propane (bisphenol A); abis(hydroxyaryl)C₄₋₁₀cycloalkane such as1,1-bis(4-hydroxyphenyl)cyclohexane; 4,4′-dihydroxydiphenyl ether;4,4′-dihydroxydiphenyl sulfone; 4,4′-dihydroxydiphenyl sulfide;4,4′-dihydroxydiphenyl ketone; and others.

The preferred poly carbonate-series resin includes a bisphenol A-basedpolycarbonate. These polycarbonate-series resins may be used singly orin combination.

(5) Polyphenylene Oxide-Series Resin

The polyphenylene oxide-series resin (polyphenylene ether-series resin)may include a homopolymer and a copolymer. As the homopolymer, there maybe mentioned a poly(mono-, di- or triC₁₋₆alkyl-phenylene) oxide, apoly(mono- or diC₆₋₂₀aryl-phenylene) oxide, and apoly(monoC₁₋₆alkyl-monoC₆₋₂₀aryl-phenylene) oxide. For example, such ahomopolymer may include a poly(2,6-dimethyl-1,4-phenylene)oxide, apoly(2,5-dimethyl-1,4-phenylene)oxide, and apoly(2,5-diethyl-1,4-phenylene)oxide.

As the copolymer of a polyphenylene oxide, there may be mentioned: acopolymer having not less than two of monomer units constituting theabove-mentioned homopolymers (e.g., a random copolymer having2,6-dimethyl-1,4-phenylene oxide unit and 2,3,6-trimethyl-1,4-phenyleneoxide unit); a modified polyphenylene oxide copolymer comprising apolyphenylene oxide block as the main structure and an alkylphenol-modified benzene formaldehyde resin block which is obtainable bya reaction of an alkyl phenol (such as cresol) with a benzeneformaldehyde resin (a formaldehyde condensate such as a phenol resin) oran alkylbenzene formaldehyde resin; a modified graft copolymer in whicha styrenic polymer and/or an unsaturated carboxylic acid or an anhydridethereof (e.g., (meth)acrylic acid, and maleic anhydride) is grafted to apolyphenylene oxide or a copolymer thereof; and others. Thesepolyphenylene oxide-series resins may be used singly or in combination.

(6) Vinyl-Series Resin

The vinyl-series resin may include a homo- or copolymer of avinyl-series monomer [e.g., a vinyl ester such as vinyl acetate; achlorine-containing vinyl monomer (e.g., vinyl chloride, andchloroprene); a fluorine-containing vinyl monomer; a vinyl ketone; avinyl ether; and a vinyl amine such as N-vinylcarbazole], or a copolymerof a vinyl-series monomer and other copolymerizable monomer. Aderivative of the above-mentioned vinyl-series resin (e.g., a polyvinylalcohol, a polyvinyl acetal such as a polyvinyl formal or a polyvinylbutyral, and an ethylene-vinyl acetate copolymer) maybe also used. Thesevinyl-series resins may be used singly or in combination.

(7) Olefinic Resin

The olefinic resin may include, for example, a homo- or copolymer of anα-C₂₋₁₀olefin (such as ethylene or propylene), a cyclic olefin-seriesresin (e.g., a homopolymer of a C₃₋₁₀cyclic olefin, and anα-C₂₋₁₀olefin-cyclic olefin copolymer), in particular, apropylene-series resin and an ethylene-series resin (e.g., apropylene-ethylene copolymer, a propylene-(meth)acrylic acid copolymer,an ethylene-ethyl(meth)acrylate copolymer, and anethylene-glycidyl(meth)acrylate copolymer).

(8) Acrylic Resin

The acrylic resin may include, for example, a homo-or copolymer of a(meth)acrylic monomer (e.g., (meth)acrylic acid or an ester thereof), inaddition a copolymer of a (meth) acrylic monomer and a copolymerizablemonomer (e.g., a (meth)acrylic acid-styrene copolymer, and amethyl(meth)acrylate-styrene copolymer).

(9) Other Resins

As other resins, there may be exemplified a polyacetal resin; a ketoneresin; a polysulfone-series resin [e.g., a polysulfone, a poly(ethersulfone), and a poly(4,4′-bisphenol ether sulfone)]; a poly(etherketone)-series resin (e.g., a poly(ether ketone), and a poly(ether etherketone); a poly(ether imide); a thermoplastic polyurethane-series resin;a thermoplastic polyimide; a polyoxybenzylene; a thermoplasticelastomer; and the like.

The preferred base resin includes a polyester-series resin which may bea liquid crystalline polyester, a styrenic resin, a polyamide-seriesresin, a polycarbonate-series resin, a polyphenylene oxide-series resin,and a vinyl-series resin, and more preferably includes apolyester-series resin, a polycarbonate-series resin, and a styrenicresin. In particular, the base resin at least containing apolyester-series resin (e.g., a PBT-series resin, and a PET-seriesresin) is preferred.

From the viewpoint of inhibition of blooming, the polyester-series resinand the styrenic resin may be used in combination. The proportion(weight ratio) of the polyester-series resin relative to the styrenicresin [the former/the latter] is about 99/1 to 50/50, preferably about95/5 to 60/40, and more preferably about 90/10 to 70/30.

The number average molecular weight of the base resin is notparticularly limited to a specific one, and is suitably selecteddepending on a kind or application of resin. For example, the numberaverage molecular weight may be selected within the range of about 5×10to 200×10⁴, preferably about 1×10⁴ to 150×10⁴, and more preferably about1×10⁴ to 100×10⁴. Moreover, in the case where the base resin is apolyester-series resin, the number average molecular weight may forexample be about 5×10³ to 100×10⁴, preferably about 1×10⁴ to 70×10⁴, andmore preferably about 1.2×10⁴ to 30×10⁴.

[Flame Retardant (A)]

The flame retardant to be used in the present invention comprises a saltof (A1) an amino group-containing triazine compound with (A2) at leastone member selected from the group consisting of a sulfuric acid and asulfonic acid. The salt may be used singly or in combination.

The amino group-containing triazine compound may include a triazinecompound having a basic nitrogen atom [e.g., a triazine compound havingan amino group (including a mono-substituted amino group (iminogroup))], for example, melamine or a derivative thereof, such as a1,3,5-triazine compound [e.g., melamine, a substituted melamine (e.g.,an alkylmelamine such as 2-methylmelamine, and guanylmelamine), amelamine condensate (e.g., melam, melem, and melon), or aco-condensation resin of melamine (e.g., a melamine-formaldehyde resin,a phenol-melamine resin, a benzoguanamine-melamine resin, and anaromatic polyamine-melamine resin); a cyanuric amide such as ammeline orammelide; and guanamine or a derivative thereof, e.g., guanamine,acetoguanamine, benzoguanamine, adipoguanamine, phthaloguanamine,CTU-guanamine, a guanamine compound having a heterocycle-containinggroup as a substituent [for example, compounds described in JapanesePatent Publication No. 41120/1972 (JP-47-41120B), e.g., a2,4-diamino-6-(2′-imidazolyl-(1′)-C₁₋₄alkyl)-s-triazine which may have aC₁₋₆alkyl group and/or a C₆₋₁₀aryl group at a ternary carbon atom of animidazole ring thereof, such as2,4-diamino-6-(2′-imidazolyl)ethyl-s-triazine]], and a variety ofaminotriazines such as a 1,2,3-triazine compound (e.g., 1,2,3-triazine,and benzo-1,2,3-triazine) and a 1,2,4-triazine compound. Incidentally,the arbitrary site(s) constituting a triazine ring (nitrogen atom andcarbon atom, particularly carbon atom) may have an amino group(s) assubstituent(s). The number of amino groups is not particularly limitedto a specific one, and for example, is about 1 to 3, and particularlyabout 2 to 3.

The preferred amino group-containing triazine compound includesmelamine, a melamine condensate [for example, melam, melem, and melon(in particular, melam and melem)], and others.

The amino group-containing triazine compound, and the sulfuric acidand/or the sulfonic acid usually form a salt through at least one aminogroup as a substituent of the triazine ring. In the case where thetriazine compound has a plurality of amino groups, all of the aminogroups may form a salt with the acid. For example, a part of the aminogroups may form a salt with the sulfuric acid and all or a part of theremaining amino group(s) may form a salt with the sulfonic acid.

Examples of the sulfuric acid may include a non-condensed sulfuric acidsuch as sulfuric acid (orthosulfuric acid) or sulfurous acid; and acondensed sulfuric acid such as pyrosulfuric acid. The preferredsulfuric acid includes orthosulfuric acid and pyrosulfuric acid(hereinafter, orthosulfuric acid or pyrosulfuric acid is sometimesreferred to as simply (pyro)sulfuric acid). The sulfuric acid may beused singly or in combination.

The sulfonic acid may include an alkanesulfonic acid (e.g.,methanesulfonic acid, ethanesulfonic acid, propanesulfonic acid,butanesulfonic acid, and ethanedisulfonic acid), an arenesulfonic acid(e.g., benzenesulfonic acid, toluenesulfonic acid, naphthalenesulfonicacid, and benzenedisulfonic acid), and others. The preferred sulfonicacid includes a C₁₋₁₀alkanesulfonic acid and a C₆₋₁₂arenesulfonic acid.The sulfonic acid may be used singly or in combination.

(Salt of Amino Group-Containing Triazine Compound with Sulfuric Acid)

The salt of the amino group-containing triazine compound with thesulfuric acid (or the sulfate of the amino group-containing triazinecompound) may include, for example, a salt of anon-condensed sulfuricacid [for example, a melamine sulfate (e.g., melamine sulfate,dimelamine sulfate, and guanylmelamine sulfate), a melamine salt of anon-condensed sulfuric acid such as melamine sulfite corresponding tothe melamine sulfate of the non-condensed sulfuric acid; and a melamsalt, a melem salt, a melon salt, a melamine-melam-melem triple (orcomplexed) salt and a guanamine salt, each corresponding to the melaminesalt of the non-condensed sulfuric acid], a salt of a condensed sulfuricacid [for example, a melamine pyrosulfate (e.g., melamine pyrosulfate,and dimelamine pyrosulfate), and a melam salt (e.g., melam pyrosulfate,and dimelam pyrosulfate), a melem salt, a melon salt, amelamine-melam-melem triple salt and a guanamine salt, eachcorresponding to the melamine pyrosulfate]. The preferred sulfateincludes a melamine (pyro) sulfate such as melamine sulfate, dimelaminesulfate, or melamine pyrosulfate; a melam (pyro)sulfate such as melamsulfate, or dimelam pyrosulfate; and a melamine-melam-melem triple saltof (pyro)sulfuric acid.

Incidentally, melamine sulfate and dimelamine sulfate (hereinafter,melamine sulfate or dimelamine sulfate is sometimes referred to assimply (di)melamine sulfate) can be obtained, for example, by methodsdescribed in Japanese Patent Application Laid-Open Nos. 231517/1996(JP-8-231517A) and 255811/1997 (JP-9-255811A), and others. For example,(di) melamine sulfate is available from Sanwa Chemical Co., Ltd. astrade name “Apinon 901”. Moreover, dimelam pyrosulfate can be obtained,for example, by a method described in Japanese Patent ApplicationLaid-Open No. 306082/1998 (JP-10-306082A), and others.

(Salt of Amino Group-Containing Triazine Compound with Sulfonic Acid)

The salt of the amino group-containing triazine compound with thesulfonic acid (or the sulfonate of the amino group-containing triazinecompound) may include a salt of an alkylsulfonic acid (a salt of analkanesulfonic acid) [for example, a melamine alkylsulfonate(alkanesulfonate) (a melamine C₁₋₆alkanesulfonate such as melaminemethanesulfonate or melamine ethanesulfonate, or a melamineC₁₋₆alkanedisulfonate corresponding thereto), and a melam salt, a melemsalt, a melon salt, a melamine-melam-melem triple salt, a guanaminesalt, an acetoguanamine salt and a benzoguanamine salt, eachcorresponding to the melamine alkanesulfonate], a salt of the aminogroup-containing triazine compound with an arylsulfonic acid (anarenesulfonic acid) [for example, a melamine arylsulfonate(arenesulfonate) (e.g., melamine benzenesulfonate, and melaminetoluenesulfonate), and a melam salt, a melem salt, a melon salt, amelamine-melam-melem triple salt, a guanamine salt, an acetoguanaminesalt and a benzoguanamine salt, each corresponding to the melaminearenesulfonate]. Among these sulfonates, the preferred one includes aC₁₋₄alkanesulfonate such as a methanesulfonate (e.g., a melamine salt, amelam salt, a melem salt, and a melamine•melam•melem triple salt), abenzenesulfonate or a p-toluenesulfonate (e.g., a melamine salt, a melamsalt, a melem salt, and a melamine melam-melem triple salt), and others.The salt of the amino group-containing triazine compound with thesulfonic acid can be obtained, for example, by methods described inJapanese Patent Application Laid-Open Nos. 511409/1998 (JP-10-511409A)and 288361/2001 (JP-2001-288361A), and others. Moreover, melammethanesulfonate is available from Nissan Chemical Industries, Ltd. as“MMS-200”.

The proportion of the amino group-containing triazine compound (A1)relative to the total amount of the sulfuric acid and the sulfonic acid(A2) is not particularly limited to a specific one, and for example, theformer/the latter (molar ratio) is about 1/5 to 5/1, preferably about1/2 to 4/1, and more preferably about 1/1 to 3/1. The equivalence ratioof an amino group contained in the amino group-containing triazinecompound relative to a salifiable site of the acid (the sulfuric acidand the sulfonic acid) is not also particularly limited to a specificone, and is, for example, about 10/1 to 1/2, preferably about 5/1 to1/1, and particularly about 4/1 to 1/1.

Moreover, in some cases, the salt of the amino group-containing triazinecompound with the sulfuric acid and/or the sulfonic acid containscomponent(s) such as a free amino group-containing triazine compound,water (adsorbed water, and crystallization water) and a solvent, andsuch components adversely affect processability, in addition,moldability (or formability) of the resin composition. In such a case,the use of the salt, as the sulfate or the sulfonate, in which an amountof a volatile matter(s) (i.e., weight loss of the salt) by heating issmall, can also inhibit the deterioration of processability andmoldability due to the components.

The weight loss of the sulfate or the sulfonate due to heating may be,for example, not more than 15% by weight (e.g., about 0.001 to 15% byweight), preferably not more than 10% by weight (e.g., about 0.001 to10% by weight), more preferably not more than 5% by weight (e.g., about0.001 to 5% by weight), and particularly not more than 3% by weight(e.g., about 0.001 to 3% by weight). Incidentally, the weight loss byheating can be, for example, represented by a ratio (% by weight) ofweight decrease or loss based on the weight of the salt at 250° C. andthat of the salt at 30° C. when the salt is heated with increasing atemperature from 30° C. to 250° C at a heating rate of 20° C./min. undera nitrogen flow by using a thermogravimetric analysis apparatus.

Incidentally, in the sulfate and the sulfonate, the volatilizationamount can be reduced by preheating under an atmospheric air or aninactive gas (e.g., helium, nitrogen, and argon) atmosphere or undersuch a gas flow. The heat treatment may be, for example, carried out byheating at a temperature of 100 to 350° C. for 0.5 to 24 hours.

The flame retardant (A) may be treated with the use of asurface-modifying agent such as an epoxy-series compound, a couplingagent (e.g., a silane-series compound, a titanate-series compound, andan aluminum-series compound) or a chromium-series compound.

Moreover, the flame retardant (A) may be coated (or coating-treated)with a coating component, for example, a metal, a glass, a cyanurate ofa triazine derivative, a thermosetting resin (e.g., a phenol resin, aurea resin, a melamine resin, an aniline resin, a furan resin, a xyleneresin, or a co-condensed resin thereof, an unsaturated polyester resin,an alkyd resin, a vinylester resin, a diallylphthalate resin, an epoxyresin, a polyurethane resin, a silicon-containing resin, and apolyimide), a thermoplastic resin, or the like. Among these coatingcomponents, usually the flame retardant is preferably coated with athermosetting resin (e.g., a phenol resin, or an epoxy resin). Forexample, a coating method for the flame retardant (A) may be referred toJapanese Patent Application Laid-Open No. 169120/2000 (JP-2000-169120A),Japanese Patent Application Laid-Open No. 131293/2001 (JP-2001-131293A),and others. In the flame retardant coated with the coating component(the coated flame retardant) (A), the proportion of the coatingcomponent is not particularly limited to a specific one, and is about0.1 to 20% by weight, preferably about 0.1 to 10% by weight (e.g., about0.1 to 8% by weight) relative to the coated flame retardant.

[Flame-Retardant Auxiliary (B)]

The flame-retardant auxiliary (B) may include (B1) an aromatic resin,(B2) a cyclic urea-series compound or a derivative thereof, (B3) anamino group-containing triazine compound, and (B4) an inorganicmetal-series compound. These flame-retardant auxiliaries may be usedsingly or in combination.

[Aromatic Resin (B1)]

The resinous flame-retardant auxiliary (or flame retardant) may includea resin containing an aromatic ring having a hydroxyl group and/or anamino group, a polyarylate-series resin, an aromatic epoxy resin, apolycarbonate-series resin, an aromatic nylon, a polyphenyleneoxide-series resin, and a polyphenylene sulfide-series resin. As thepolyphenylene oxide-series resin and the polycarbonate-series resin, aresin similar to the resin exemplified in the paragraph of the baseresin may be used. The aromatic resin to be employed is usuallydifferent from the base resin.

(1) Resin Containing Aromatic Ring Having Hydroxyl group and/or AminoGroup

The aromatic ring may be located in a main chain or a side chain. Forexample, examples of a resin having the aromatic ring in a main chainthereof may include a novolak resin, and an aralkyl resin. The resinhaving the aromatic ring in a side chain thereof may include an aromaticvinyl resin.

(1-1) Novolak Resin

The novolak resin has a repeating unit represented by the followingformula (1):

wherein R¹ to R³ are the same or different, each representing a hydrogenatom, an alkyl group, or an aryl group, “r” denotes an integer of notless than 1.

The alkyl group and the aryl group may include a C₁₋₂₀alkyl group suchas methyl, ethyl, butyl or hexyl group (particularly, a C₁₋₁₂alkylgroup), a C₆₋₂₀aryl group such as phenyl group, and a substituted arylgroup (particularly a C₁₋₄alkyl-substituted aryl group).

The novolak resin (particularly a random novolak resin) is usuallyobtainable by a reaction of a phenol compound with an aldehyde. As thephenol compound, for example, there may be mentioned phenol, cresol,xylenol, an alkyl phenol (e.g., a C₁₋₂₀alkyl phenol such as t-butylphenol or p-octyl phenol), a C₆₋₁₀aryl phenol (e.g., phenyl phenol), aC₆₋₁₀aryl-C₁₋₄alkyl-phenol (e.g., benzyl phenol), and others. Thesephenol compounds may be used singly or in combination.

The aldehyde may include, for example, an aliphatic aldehyde such asformaldehyde, and an aromatic aldehyde such as phenylacetaldehyde.Moreover, a condensate of formaldehyde such as trioxane orparaformaldehyde may be also used. The ratio of the phenol compoundrelative to the aldehyde (the former/the latter) is about 1/0.5 to 1/1(molar ratio).

The condensation reaction of the phenol compound with the aldehyde isusually carried out in the presence of an acid catalyst [for example, aninorganic acid (e.g., hydrochloric acid, a sulfuric acid, and aphosphoric acid), and an organic acid (e.g., p-toluenesulfonic acid, andoxalic acid)]. In particular, it is preferred to use a phenol novolakresin having decreased content of a monomer or dimer of a phenolcompound. Such a phenol novolak resin is, for example, available astrade name “SUMILITE RESIN PR-53647”, “SUMILITE RESIN PR-NMD-100series”, or“SUMILITE RESIN PR-NMD-200 series” from Sumitomo Durez Co.,Ltd.

Moreover, as the novolak resin, a high-orthonovolak resin having anortho/para ratio of not less than 1 may be used. In particular, as thenovolak resin, it is preferred to use a novolak resin having anortho/para ratio of not less than 1, for example, about 1 to 20(particularly about 1 to 15), so-called a high-orthonovolak resin. Sucha high-orthonovolak resin is procurable from Sumitomo Durez Co., Ltd. as“SUMILITE RESIN HPN SERIES”.

The process for producing these novolak resins may be referred toJapanese Patent Application Laid-Open No. 172348/2001 (JP-2001-172348A),Japanese Patent Application Laid-Open No. 273133/2000 (JP-2000-273133A),and others.

Incidentally, there may be also used a co-condensate of theabove-mentioned phenol compound with a co-condensable component such asa dioxybenzene compound, a naphthol compound, a bisphenol compound(e.g., a bisphenol compound such as bisphenol A or bisphenol D), analkylbenzene (e.g., toluene, and xylene), an aniline compound, afurfural compound, a urea compound or a triazine compound (e.g., urea,cyanuric acid, melamine, and guanamine), a terpene compound, a cashewnut, and a rosin.

Moreover, a modified novolak resin-may be also employed, and the resinmay include a novolak resin in which phenolic hydroxyl groups arepartially or wholly modified with at least one compound selected fromphosphorus-containing compounds (e.g., a phosphoric acid compound suchas phosphoric acid, and an acid anhydride, halide, salt or ester (inparticular, an aliphatic ester) thereof) and boron-containing compounds(e.g., a boric acid compound, and an acid anhydride, halide, salt orester thereof), for example, a phosphoric acid-modified novolak resin,and a boric acid-modified novolak resin.

Further, a modified novolak resin being a novolak resin (random novolakresin and high-ortho novolak resin) in which the hydrogen atom of thephenolic hydroxyl group is partially or wholly modified (or substituted)with a metal ion, a silyl group, an organic group (e.g., an alkyl group,an alkylcarbonyl group, an arylcarbonyl group (such as benzoyl group)and a (poly)alkylene oxide group) is also available.

Preferred as the novolak resins are, for example, phenol-formaldehydenovolak resin, an alkylphenol-formaldehyde novolak resin (e.g., acresol-formaldehyde novolak resin, a t-butylphenol-formaldehyde novolakresin, a p-octylphenol-formaldehyde resin, and a xylenol-formaldehydenovolak resin), a co-condensate thereof (an aminotriazine-novolak resinin which a novolak resin is modified with a triazine compound such asmelamine) and a modified resin thereof [an alkylene oxide adduct polymerin which a C₁₋₄alkylene oxide (such as ethylene oxide or propyleneoxide) is added to a novolak resin], and a mixture thereof. Theaminotriazine-novolak resin is, for example, from Dainippon Ink AndChemicals, Inc. as trade name “PHENOLITE”.

There is no particular restriction as to the number average molecularweight of the novolak resin, and it may be selected within the range of300 to 5×10⁴, and preferably 300 to 1×10⁴.

(1-2) Aralkyl Resin

The aralkyl resin has a structural unit represented by the followingformula (2):

wherein Ar represents an aromatic group, Z¹ and Z² are the same ordifferent, each representing an alkylene group, R⁴ represents a hydrogenatom or an alkyl group, and X represents a hydroxyl group, an aminogroup, or an N-substituted amino group.

The aromatic group represented by Ar may include a C₆₋₂₀arylene group(e.g., a phenylene group, and a naphthylene group). Among them, thephenylene group (particularly p-phenylene group) is preferred. Thealkylene group represented by Z¹ and Z² may include a C₁₋₄alkylene groupsuch as methylene group or ethylene group. The alkyl group representedby R⁴ may include a C₁₋₄alkyl group such as methyl group or ethyl group.The N-substituted amino group represented by X may include a mono- ordiC₁₋₄alkylamino group (e.g., dimethylamino group, and diethylaminogroup).

As the aralkyl resin, a phenol aralkyl resin in which X is a hydroxylgroup is used practically. The preferred phenol aralkyl resin mayinclude a resin having methylene groups as Z¹ and Z², a phenylene groupas Ar, a hydrogen atom as R⁴ in the above formula (2), and having ap-xylene-substituted phenol represented by the following formula (3) asa repeating unit.

The aralkyl resin may be usually obtained by reacting a compoundrepresented by the following formula (4) with a phenol compound or ananiline compound.Y-Z¹-Ar-Z²-Y   (4)

In the formula, Y represents an alkoxy group, an acyloxy group, ahydroxyl group, or a halogen atom, and Ar, Z¹ and Z² have the samemeanings as defined above.

In the formula (4), an alkoxy group represented by Y may include aC₁₋₄alkoxy group such as methoxy or ethoxy group. Examples of theacyloxy group may include an acyloxy group having about 2 to 5 carbonatoms. Moreover, examples of the halogen atom may include chlorine,bromine, and others.

The compound represented by the formula (4), for example, may include anaralkyl ether such as a xylylene glycol C₁₋₄alkyl ether (e.g.,p-xylylene glycol dimethyl ether), an acyloxyaralkyl compound such asp-xylylene-α,α′-diacetate, an aralkyldiol such as p-xylylene-α,α′-diol,an aralkyl halide such as p-xylylene-α,α′-dichloride orp-xylylene-α,α′-dibromide. The phenol compound may include a phenolcompound or an alkylphenol compound which are exemplified in the sectionon the novolak resin. These phenol compounds may be used either singlyor in combination.

Examples of the aniline compound may include aniline, an alkylaniline(e.g., a C₁₋₂₀alkylaniline such as toluidine or octylaniline), and anN-alkylaniline (e.g., N,N-dimethylaniline). These aniline compounds maybe used either singly or in combination.

The ratio of the compound represented by the formula (4) relative to thephenol compound or the aniline compound (the former/the latter) is, forexample, about 1/1 to 1/3 (molar ratio), and preferably about 1/1 to1/2.5 (molar ratio).

The softening point of the aralkyl resin thus obtained is, for example,about 40 to 160° C., preferably about 50 to 150° C., and more preferablyabout 55 to 140° C. Incidentally, as other aralkyl resin, there may beused an aralkyl resin described in Japanese Patent Application Laid-OpenNo. 351822/2000 (JP-2000-351822A).

If necessary, the aralkyl resin may be cured or modified. Curing ormodification may be usually effected by a conventional method, such asaddition polymerization with an alkylene oxide (e.g., ethylene oxide,and propylene oxide), methylene-crosslinking with the use of a polyamine(e.g., hexamethylenetetramine) or epoxy-modification with the use of anepoxy compound (e.g., epichlorohydrin).

(1-3) Aromatic Vinyl Resin

The aromatic vinyl resin may include, for example, a resin having astructural unit represented by the following formula (5):

wherein R⁵ represents a hydrogen atom or a linear or branched C₁₋₃alkylgroup, R⁶ represents an aromatic ring, and “s” denotes an integer of 1to 3.

In the formula (5), the C₁₋₃alkyl group may include methyl group, andothers. As the aromatic ring, there may be mentioned a C₆₋₂₀aromaticring such as benzene ring or naphthalene ring. Incidentally, thearomatic ring may have a substituent (e.g., a hydroxyl group; the alkylgroup exemplified in the item on the above-mentioned R¹ to R³; thealkoxy group exemplified in the item on the above-mentioned Y).

In the formula (5), the hydroxyl group may be protected by a protectinggroup such as a metal ion, a silyl group, or an organic group (e.g., analkyl group, an alkylcarbonyl group, and an arylcarbonyl group (such asbenzoyl group)). Moreover, to the hydroxyl group may be added analkylene oxide (e.g., ethylene oxide, and propylene oxide).

A resin obtained from such a derivative has, for example, a structuralunit represented by the following formula (6):

wherein R⁵ has the same meaning as defined above; R⁷ is a group selectedfrom the group consisting of —OH, —OM (M represents a metal cation),—OSi(R⁸)₃, —OR⁸, —OC(═O)R⁸ (R⁸ represents a C₁₋₆alkyl group or aC₆₋₂₀aryl group) and —O(A¹O)_(u)H (A¹ represents a C₁₋₄alkylene group,the repeating number “u” is an integer of 1 to 5); and “t” denotes aninteger of 1 to 3.

In the formula (6), the metal cation “M” may be any one of a monovalentcation of an alkali metal (e.g., sodium, lithium, and potassium), abivalent cation of an alkaline earth metal (e.g., magnesium, andcalcium), or a transition metal cation.

In the formula (6), it is sufficient that the substituent R⁷ ispositioned in any one of ortho-position, meta-position or para-positionto the main chain. Further, in addition to the substituent R⁷, a pendantaromatic ring may have a C₁₋₄alkyl group as a substituent.

The aromatic vinyl-series resin may include a homo- or copolymer of anaromatic vinyl monomer having a hydroxyl group (e.g., a hydroxylgroup-containing monomer such as vinyl phenol or dihydroxystyrene),corresponding to the above-mentioned structural unit (5), or a copolymerwith other copolymerizable monomer. These monomers may be used singly orin combination.

Examples of the other copolymerizable monomer include a (meth)acrylicmonomer [e.g., (meth)acrylic acid, a (meth)acrylate, (meth)acrylamide,and (meth)acrylonitrile], a styrenic monomer, a polymerizablepolycarboxylic acid, a maleimide-series monomer, a diene-series monomer,and a vinyl-series monomer (e.g., a vinyl ester such as vinyl acetate; avinyl ketone; a vinyl ether; and a nitrogen-containing vinyl monomersuch as N-vinylpyrrolidone). These copolymerizable monomers may be usedeither singly or in combination.

The ratio of the vinyl monomer relative to the copolymerizable monomeris, for example, about 10/90 to 100/0 (% by weight), preferably about30/70 to 100/0 (% by weight), and more preferably about 50/50 to 100/0(% by weight).

The preferred aromatic vinyl resin includes a vinylphenol homopolymer (apolyhydroxystyrene), particularly a p-vinylphenol homopolymer.

There is no particular restriction as to the number average molecularweight of the aromatic vinyl-series resin, and it may be selected withinthe range of, for example, 300 to 50×10⁴, and preferably 400 to 30×10⁴.

(2) Polyarylate-Series Resin

The polyarylate-series resin has a structural unit represented by thefollowing formula (7):[—O—Ar—OC(O)-A²-C(O)—]  (7)

wherein Ar stands for an aromatic group and A² stands for an aromatic,alicyclic, or aliphatic group.

The polyarylate-series resin may be obtained by a conventionalpolyesterification reaction, for example, a reaction between an aromaticpolyol component and an polycarboxylic acid component (e.g., an aromaticpolycarboxylic acid component, an aliphatic polycarboxylic acidcomponent (the aliphatic dicarboxylic acid exemplified in the paragraphof the above-mentioned polyester-series resin (a C₂₋₂₀aliphaticdicarboxylic acid such as adipic acid)), and an alicyclic polycarboxylicacid component (a C₃₋₂₀alicyclic dicarboxylic acid such ascyclohexanedicarboxylic acid)). The polycarboxylic acid componentusually contains at least the aromatic polycarboxylic acid component.

As the aromatic polyol (monomer), a diol such as a monocyclic aromaticdiol or a polycyclic aromatic diol, or a reactive derivative thereof maybe usually employed. These aromatic polyols may be used singly or incombination.

Examples of the monocyclic aromatic diol may include an aromatic diolhaving about 6 to 20 carbon atoms, such as a benzenediol, xylyleneglycol or naphthalenediol. The polycyclic aromatic diol may include abis(hydroxyaryl) (a bisphenol compound), for example, abis(hydroxyaryl)C₁₋₆alkane such as 4,4′-dihydroxybiphenyl,2,2′-biphenol, bisphenol A, bisphenol D or bisphenol F; and abis(hydroxyaryl)C₃₋₁₂cycloalkane. Moreover, the polycyclic aromatic diolmay also include a compound having a bis(hydroxyaryl) backbone, such asdi(hydroxyphenyl) ether, di(hydroxyphenyl)ketone,di(hydroxyphenyl)sulfoxide, and in addition, di(hydroxyphenyl)thioether,a bis(C₁₋₄alkyl-substituted hydroxyphenyl)alkane and a terpene diphenolcompound.

The preferred aromatic polyol includes a benzenediol compound and abisphenol compound [for example, a bis(hydroxyaryl)C₁₋₆alkane (e.g.,bisphenol A, bisphenol F, and bisphenol AD)].

Incidentally, the aromatic polyol may be used together with an aliphaticpolyol (a C₂₋₁₀alkylene glycol) or an alicyclic polyol (a polyol havinga C₃₋₁₀aliphatic ring, such as 1,4-cyclohexanedimethanol orcyclohexanediol).

Examples of the aromatic polycarboxylic acid may include a monocyclicaromatic dicarboxylic acid, a polycyclic aromatic dicarboxylic acid, ora reactive derivative thereof (for example, an aromatic polycarboxylicacid halide, an aromatic polycarboxylic ester, and an aromaticpolycarboxylic acid anhydride).

The monocyclic aromatic dicarboxylic acid may include abenzenedicarboxylic acid such as phthalic acid, phthalic anhydride,isophthalic acid, or terephthalic acid, and an aryldicarboxylic acidhaving carbon atoms of about 8 to 20 (such as naphthalenedicarboxylicacid). Incidentally, the benzenedicarboxylic acid and thenaphthalenedicarboxylic acid (particularly, benzenedicarboxylic acid)may have one or two C₁₋₄alkyl group(s) as a substituent. Examples of thepolycyclic aromatic dicarboxylic acid may include a bis (arylcarboxylicacid), for example, biphenyldicarboxylic acid, abis(carboxyaryl)C₁₋₆alkane; a bis(carboxyaryl)C₃₋₁₂cycloalkane; and abis(carboxyaryl)ether.

The preferred aromatic polycarboxylic acid component includes themonocyclic aromatic dicarboxylic acid (particularly, abenzenedicarboxylic acid such as phthalic acid, isophthalic acid orterephthalic acid), the bis(carboxyaryl)C₁₋₆alkane, and others.

If necessary, an aromatic triol, an aromatic tetraol, an aromatictricarboxylic acid, an aromatic tetracarboxylic acid, or the like maybeused in combination with the aromatic diol and the aromatic dicarboxylicacid.

The preferred polyarylate-series resin includes a polyarylate-seriesresin in which the aromatic polyol is a bisphenol compound and/or abenzenediol compound, for example, a polyester of a bisphenol compound(e.g., bisphenol A) and/or a benzenediol compound (e.g., resorcinol) anda benzenedicarboxylic acid (e.g., terephthalic acid), a polyester of abisphenol compound and/or a benzenediol compound and abis(arylcarboxylic acid) [e.g., a bis(carboxyaryl)C₁₋₄alkyl such asbis(carboxyphenyl)propanel, and others. These polyarylate-series resinsmay be used singly or in combination.

The terminal (or end) of the polyarylate-series resin may be blocked orcapped with (bonded to) an alcohol (e.g., an alkyl alcohol, an arylalcohol, and an aralkyl alcohol), or a carboxylic acid (e.g., analiphatic carboxylic acid, an alicyclic carboxylic acid, and an aromaticcarboxylic acid).

The number average molecular weight of the polyarylate-series resin is,for example, about 300 to 30×10⁴, preferably about 500 to 10×10⁴, andmore preferably about 500 to 5×10⁴.

(3) Aromatic Epoxy Resin

Examples of the aromatic epoxy resin may include an ether-series epoxyresin (e.g., a bisphenol-based epoxy resin, and a novolak epoxy resin),and an amine-series epoxy resin formed with an aromatic amine component.

Examples of the bisphenol constituting a bisphenol-based epoxy resin aresimilar to the bis(hydroxyaryl) listed above. The preferredbisphenol-based epoxy resin may include a glycidyl ether of abis(hydroxyaryl)C₁₋₆alkane, particularly bisphenol A, or the like.Moreover, examples of the bisphenol-based epoxy resin also include aresin having a high molecular weight (that is, a phenoxy resin).

Examples of the novolak resin constituting a novolak epoxy resin mayinclude a novolak resin in which an alkyl group (e.g., a C₁₋₄ alkylgroup such as methyl group) may be substituted on the aromatic ring(e.g., a phenol-novolak resin, and a cresol-novolak resin).

Examples of the aromatic amine component constituting an amine-seriesepoxy resin may include a monocyclic aromatic amine (e.g., aniline), amonocyclic aromatic diamine (e.g., diaminobenzene), a monocyclicaromatic aminoalcohol (e.g., aminohydroxybenzene), a polycyclic aromaticdiamine (e.g., diaminodiphenylmethane), and a polycyclic aromatic amine.

The number average molecular weight of the epoxy resin is, for example,about 200 to 50,000, preferably about 300 to 10,000, and more preferablyabout 400 to 6,000 (e.g., about 400 to 5,000). Moreover, the numberaverage molecular weight of the phenoxy resin is, for example, about 500to 50,000, preferably 1,000 to 40,000, and more preferably about 3,000to 35,000.

The epoxy resin may be used in a cured state, and the curing is effectedby the use of a curing agent, e.g., an amine-series curing agent (e.g.,an aliphatic amine such as ethylenediamine, and an aromatic amine suchas metaphenylenediamine), a polyaminoamide-series curing agent, an acidand acid anhydride-series curing agent.

These resin components may be used singly or in combination.

(4) Aromatic Nylon

As the aromatic nylon constituting the flame retardant, a resindifferent in kind from the polyamide resin of the base resin is used. Assuch a resin, there may be used a compound having a unit represented bythe following formula (8):

wherein Z³ and Z⁴ are the same or different, each selecting from analiphatic hydrocarbon group, an alicyclic hydrocarbon group, and anaromatic hydrocarbon group, and at least one of Z³ and Z⁴ is an aromatichydrocarbon group; R⁹ and R¹⁰ are the same or different, each selectingfrom a hydrogen group, an alkyl group, and an aryl group; or R⁹ and R¹⁰may be connected directly with each other to form a ring.

Such an aromatic nylon may include a polyamide derived from a diamineand a dicarboxylic acid, in which at least one component of the diaminecomponent and the dicarboxylic acid component is an aromatic compound;and a polyamide obtained from an aromatic aminocarboxylic acid, and ifnecessary a diamine and/or a dicarboxylic acid in combination. Thearomatic nylon may also include a copolyamide.

The diamine may include, for example, an aromatic diamine such asphenylenediamine, xylylenediamine (in particular, metaxylylenediamine,paraxylylenediamine), a diamine having a biphenyl backbone, a diaminehaving a diphenylalkane backbone, or 1,4-naphthalenediamine, and anN-substituted aromatic diamine thereof. Moreover, the aromatic diaminemay be used in combination with an alicyclic diamine, an aliphaticamine, and an N-substituted aliphatic diamine thereof, and others. Thesediamines may be used singly or in combination. As the diamine, it ispreferred to use an aromatic diamine (in particular xylylenediamine,N,N′-dialkyl-substituted xylylenediamine).

The dicarboxylic acid may include, for example, a C₂₋₂₀aliphaticdicarboxylic acid such as adipic acid, suberic acid, sebacic acid, ordodecanedicarboxylic acid; an aromatic dicarboxylic acid such asphthalic acid, or naphthalenedicarboxylic acid; an alicyclicdicarboxylic acid such as cyclohexanedicarboxylic acid; and a dimerizedfatty acid. These dicarboxylic acids may be used singly or incombination. As the dicarboxylic acid, it is preferred to use analiphatic dicarboxylic acid (in particular a C₆₋₂₀aliphatic dicarboxylicacid such as adipic acid).

As the aromatic or alicyclic aminocarboxylic acid, there may beexemplified phenylalanine, aminobenzoic acid, or the like. Theseaminocarboxylic acids may be also used singly or in combination.

Moreover, as the aromatic nylon, a condensate of a lactam and/or anα,ω-aminocarboxylic acid may be used insofar as characteristics of aflame retardant is not deteriorated.

The accessory ingredient of the aromatic nylon may include a monobasicacid (for example, acetic acid), a monoamine (for example, butylamine,and benzylamine), a dibasic acid (for example, adipic acid, sebacicacid, terephthalic acid, and isophthalic acid), a diamine (for example,tetramethylenediamine, hexamethylenediamine), a lactam or others, and atleast one member selected therefrom may be used as a viscosityadjustment (or viscosity controller).

The aromatic nylon may include a polyamide or copolyamide comprising anaromatic diamine (e.g., xylylenediamine) as a diamine component,preferably a polyamide obtained from an α,ω-C₆₋₁₂dicarboxylic acid andan aromatic diamine (e.g., metaxylylenediamine, paraxylylenediamine,N,N′-dimethylmetaxylylenediamine, 1,3-phenylenediamine, and4,4′-diaminodiphenylmethane) [for example, a polyamide obtained fromadipic acid and a xylylenediamine (e.g., MXD6, and PMD6), and apolyamide obtained from suberic acid and instead of adipic acid]. Thesepolyamides may be used singly or in combination.

The aromatic nylon is prepared by a direct method under atmosphericpressure or a melt polymerization based on, for example, Japanese PatentApplication Laid-Open No. 283179/1987 (JP-62-283179A), KogyokagakuZasshi (Journal of the Chemical Society of Japan, Industrial Chemistry)Vol. 74, No. 4, page 786 (1971), Engineering Plastic Jiten (EngineeringPlastic Dictionary) page 74 (Gihodo Shuppan Co., Ltd., 1998), andreferences described in these documents.

The number average molecular weight of the aromatic nylon is notparticularly limited to a specific one, and for example may be selectedfrom the range of about 300 to 10×10⁴, and preferably about 500 to5×10⁴.

(5) Polyphenylene Sulfide-Series Resin

The polyphenylene sulfide-series resin (polyphenylene thioether-seriesresin) may include a homopolymer or copolymer having a polyphenylenesulfide backbone, —(Ar—S—)— (wherein Ar represents a phenylene group).As the phenylene group (—Ar—), there may be mentioned, for example, p-,m-, or o-phenylene group, a substituted phenylene group (e.g., analkylphenylene group having substituent(s) such as a C₁₋₅alkyl group, anarylphenylene group having substituent(s) such as phenyl group),—Ar-A³-Ar— [wherein Ar represents a phenylene group, and A³ represents adirect bond between the two Ar groups, or O, CO or SO₂]. Thepolyphenylene sulfide-series resin may be a homopolymer obtained from ahomogeneous repeating unit among the phenylene sulfide groups comprisingsuch a phenylene group, or in view of workability of the composition,may be a copolymer containing a heterogeneous repeating unit among thephenylene sulfide groups comprising such a phenylene group.

As the homopolymer, a substantially linear polymer comprisingp-phenylene sulfide group as a repeating unit is preferably used. Thecopolymer may be obtained from two or more different kinds of phenylenesulfide groups among the phenylene sulfide groups. Among others, acopolymer comprising p-phenylene sulfide group as a main repeating unitin combination with m-phenylene sulfide group is preferred. From theviewpoint of physical properties such as heat resistance, moldability,and mechanical property, a substantially linear copolymer comprising notless than 60 mol % (preferably 70 mol %) of p-phenylene sulfide group isparticularly preferred.

The polyphenylene sulfide resin may be a polymer obtained by allowing arelative low molecular weight of a linear polymer to crosslink withoxidation or heating for increasing the melt viscosity of the polymerthereby improving molding processability (mold-processability), or ahigh molecular weight polymer having a substantially linear structurewhich polymer is obtained by condensation polymerization from a monomermainly comprising a bifunctional monomer. From the viewpoint of physicalproperties of the resultant shaped article, a polymer having asubstantially linear structure, which is obtained by condensationpolymerization is more preferred. Moreover, as the polyphenylene sulfideresin, in addition to the above-mentioned polymer, a branched orcrosslinked polyphenylene sulfide resin obtained by a polymerization ofthe monomer in combination with a monomer having not less than three offunctional groups, or a resin-composition obtained by blending the resinto the above-mentioned linear polymer may be also used.

As the polyphenylene sulfide-series resin, there may be used apolyphenylene sulfide or a polybiphenylene sulfide (PBPS), in addition apolyphenylene sulfide ketone (PPSK), a polybiphenylene sulfide sulfone(PPSS), or others. These polyphenylene sulfide-series resins may be usedsingly or in combination.

The number average molecular weight of the polyphenylene sulfide-seriesresin is, for example, about 300 to 30×10⁴, and preferably about 400 to10×10⁴.

(B2) Cyclic Urea-Series Compound or Derivative Thereof

The cyclic urea-series compound comprises at least one urea unit—NHCONH— (including isomers of the urea unit, e.g., —N═C(OH)NH— or—NHC(OH)═N—) as a constituent unit of a ring thereof, and may be any ofa monocyclic compound, and a condensed ring or crosslinked ring with anaromatic hydrocarbon ring. The cyclic urea-series compound may include acyclic ureide (e.g., a cyclic monoureide having one urea unit as aconstituent unit of a ring thereof, and a cyclic diureide having twourea units as a constituent unit of a ring thereof). Further, the cyclicurea-series compound may also include a cyclic thiourea compoundcorresponding to the above-mentioned cyclic urea. These cyclic ureacompounds may be used singly or in combination.

As the cyclic monoureide, for example, there may be mentioned analkyleneurea [e.g., a C₁₋₁₀alkyleneurea such as methyleneurea,ethyleneurea or crotonylideneurea (CDU) (preferably, aC₁₋₆alkyleneurea)], an alkenyleneurea (e.g., a C₂₋₁₀alkenyleneurea suchas vinyleneurea or cytosine), an alkynyleneurea [e.g., aC₂₋₁₀alkynyleneurea (preferably, a C₂₋₆alkynyleneurea)], an aryleneurea,a ureide of a dicarboxylic acid (e.g., parabanic acid, dimethylparabanicacid, barbituric acid, 5,5-diethylbarbituric acid, dilituric acid,dialuric acid, alloxan, alloxanic acid, cyanuric acid, isocyanuric acid,and uramil), a ureide of a β-aldehydic acid (e.g., uracil,5-methyluracil (thymine), dihydrouracil, urazole, and benzoyleneurea), aureide of an α-hydroxy acid [e.g., a hydantoin compound such ashydantoin or 5,5-dimethylhydantoin], or a derivative thereof.

As the cyclic diureide, for example, there may be mentioned uric acid,3-methyluric acid, pseudouric acid, acetyleneurea (glycoluril), adiureide of a α-hydroxy acid [e.g.,1,1-methylenebis(5,5-dimethylhydantoin), and allantoin], a diurea suchas p-urazine, a diureide of a dicarboxylic acid (e.g., alloxantin, andpurpuric acid), or a derivative thereof.

The acetyleneurea or a derivative thereof may include, for example, acompound represented by the following formula (9). The uric acid or aderivative thereof may include, for example, a compound represented bythe following formula (10).

Wherein R¹¹ to R¹⁸ are the same or different and each represents ahydrogen atom, an alkyl group, an alkenyl group, an alkoxy group, anacyl group, an acyloxy group, a cycloalkyl group, an aryl group, anarylalkyl group, and others.

The alkyl group may include a C₁₋₈(preferably a C₁₋₄)alkyl group, thealkenyl group may include a C₂₋₈(preferably a C₂₋₄)alkenyl group, andthe alkoxy group may include a C₁₋₈ (preferably a C₁₋₄)alkoxy group. Theacyl group may include a C₁₋₈(preferably a C₁₋₄)acyl group, the acyloxygroup may include a C₁₋₈(preferably a C₁₋₄)acyloxy group, and thecycloalkyl group may include a C₅₋₁₆(preferably a C₅₋₈)cycloalkyl group.The aryl group may include a C₆₋₁₂(preferably a C₆₋₁₀)aryl group, andthe arylalkyl group may include a C₆₋₁₂(preferably aC₆₋₁₀)aryl-C₁₋₈(preferably C₁₋₄)alkyl group. As the acetyleneurea, uricacid, or a derivative thereof, a compound in which R¹¹ to R¹⁸ representa hydrogen atom or a C₁₋₄alkyl group such as methyl group (e.g.,acetyleneurea, uric acid, and 3-methyluric acid) is preferred.

Examples of the cyclic thiourea may include ethylenethiourea,thiobarbituric acid, dithiourazole, thiohydantoin, dithiohydantoin, andothers.

Moreover, the cyclic urea-series compound (in particular, a cyclicmonoureide, or a cyclic diureide) also includes a salt. The salt is notparticularly limited to a specific one as long as the cyclic urea-seriescompound or a derivative thereof can form the salt. For example, thesalt may include a salt of the cyclic urea-series compound with at leastone member selected from the group consisting of the aminogroup-containing triazine compound exemplified in the paragraph of theflame retardant (A) (e.g., an amino group-containing triazine compoundsuch as melamine or a melamine condensate), a sulfuric acid, a sulfonicacid, a boric acid, and a metal (e.g., an alkali metal, an alkalineearth metal, zinc, aluminum, and a transition metal). In particular, asalt thereof with the triazine compound is preferred. These salts may beused singly or in combination.

The preferred salt with the triazine compound may include, for example,a salt of acetyleneurea, uric acid, cyanuric acid or isocyanuric acidwith a melamine compound (e.g., at least one member selected from thegroup consisting of melamine, melem, melam, melon, and guanamine);particularly, a melamine salt of cyanuric acid (melamine cyanurate), amelem salt, a melam salt, a melon salt and a guanamine salt, eachcorresponding to the melamine salt of cyanuric acid (e.g., guanaminecyanurate, acetoguanamine cyanurate, and benzoguanamine cyanurate); amelamine salt of acetyleneurea, and a melem salt, a melam salt, a melonsalt and a guanamine salt, each corresponding to the melamine salt ofacetyleneurea.

The proportion of the cyclic urea-series compound relative to thesalt-forming (salifiable) component is not particularly limited to aspecific one, and for example, the former/the latter (molar ratio) isabout 1/5 to 4/1, preferably about 1/3 to 2/1, and more preferably about1/2 to 1/1.

Among these cyclic urea-series compounds, a salt of acetyleneurea, uricacid, melamine or a condensate thereof (e.g., melam, melem, and melon)with cyanuric acid is preferred.

(B3) Amino Group-Containing Triazine Compound

The amino group-containing triazine compound as the flame-retardantauxiliary (B) may include the amino group-containing triazine compoundmentioned in the paragraph of the flame retardant (A). The aminogroup-containing triazine compound (B3) may be used singly or incombination. Among the amino group-containing triazine compounds, thepreferred one includes melamine or a derivative thereof [e.g., amelamine condensate such as melamine, melem, or melon (particularlymelam and melem)], and guanamine or a derivative thereof [e.g.,acetoguanamine, benzoguanamine, adipoguanamine, phthaloguanamine,CTU-guanamine, and a guanamine compound having a heterocycle-containinggroup as a substituent (e.g.,2,4-diamino-6-(2′-imidazolyl-(1′)-alkyl)-s-triazine)].

(B4) Inorganic Metal-Series Compound

The inorganic metal-series compound (B4) may include a metal salt of aninorganic acid, a metal oxide, a metal hydroxide, a metal sulfide, andothers. The inorganic metal compound may be any one of an anhydride or ahydrous compound. These inorganic metal compounds may be used singly orin combination. As the inorganic metal compounds, the preferred oneincludes a metal salt of an inorganic acid (e.g., a metal borate, ametal hydrogen phosphate, a metal stannate, a metal molybdate, and ametal tungstate), a metal oxide, a metal hydroxide, and a metal sulfide.Incidentally, the inorganic metal compound does not include anyinorganic filler in practical cases.

As the inorganic acid constituting the metal salt of the inorganic acid,there may be used an oxygen acid having no sulfur atom (excluding acarbonic acid) such as a boric acid, a phosphoric acid, a stannic acid,a molybdic acid, or a tungstic acid. The oxygen acid having no sulfuratom (or sulfur-free oxygen acid) may be a polyacid (e.g., a polyacidcontaining a metal of the group 5 or 6 of the Periodic Table ofElements). The polyacid may include, for example, an isopolyacid such asisopolychromic acid; a heteropolyacid such as cobaltmolybdate,cobalttungstate, molybdenumtungstate, vanadiummolybdate, orvanadomolybdophosphate.

The metal forming a salt with the inorganic acid may include an alkalimetal (e.g., potassium, and sodium); an alkaline earth metal (e.g.,magnesium, and calcium); a transition metal [e.g., the metal of theGroup 3A of the Periodic Table of Elements (such as scandium); the metalof the Group 4A of the Periodic Table of Elements (such as titanium);the metal of the Group 5A of the Periodic Table of Elements (such asvanadium); the metal of the Group 6A of the Periodic Table of Elements(such as chromium or molybdenum); the metal of the Group 7A of thePeriodic Table of Elements (such as manganese); the metal of the Group 8of the Periodic Table of Elements (such as iron, cobalt, or nickel); andthe metal of the Group 1B of the Periodic Table of Elements (such ascopper or silver)], the metal of the Group 2B of the Periodic Table ofElements (such as zinc), the metal of the Group 3B of the Periodic Tableof Elements (such as aluminum), the metal of the Group 4B of thePeriodic Table of Elements (such as tin), and the metal of the Group 5Bof the Periodic Table of Elements (such as antimony). These metals maybe used singly or in combination.

(Metal Borate)

The boric acid may preferably include a non-condensed boric acid such asorthoboric acid or metaboric acid; a condensed boric acid such aspyroboric acid, tetraboric acid, pentaboric acid or octaboric acid; anda basic boric acid. As the metal, the alkali metal may be used, and itis preferred to use a polyvalent metal such as the alkaline earth metal,the transition metal or the metal of the Group 2B of the Periodic Tableof Elements.

The metal borate is usually a hydrous salt and may include, for example,a non-condensed borate [e.g., a non-condensed borate of an alkalineearth metal (such as calcium orthoborate or calcium metaborate);anon-condensed borate of a transition metal (such as manganeseorthoborate or copper metaborate); a non-condensed borate of the metalof the Group 2B of the Periodic Table of Elements (such as zincmetaborate), in particular metaborate], a condensed borate [e.g., acondensed borate of an alkaline earth metal (such as trimagnesiumtetraborate or calcium pyroborate); a condensed salt of a transitionmetal (such as manganese tetraborate or nickel diborate); a condensedborate of the metal of the Group 2B of the Periodic Table of Elements(such as zinc tetraborate or cadmium tetraborate)], and a basic borate(e.g., a basic borate of the metal of the Group 2B of the Periodic Tableof Elements, such as basic zinc borate). Moreover, a hydrogenboratecorresponding to the borate (e.g., manganese hydrogenorthoborate) may bealso employed. In particular, a borate of the alkaline earth metal ormetal of the Group 2B of the Periodic Table of Elements (a non-condensedor condensed borate), particularly a (hydrous) zinc borate, a (hydrous)calcium borate, is preferred.

(Metal phosphate)

The phosphoric acid may include a non-condensed phosphoric acid such asorthophosphoric acid, metaphosphoric acid, phosphorous acid, orhypophosphorous acid; and a condensed phosphoric acid such ashypophosphoric acid , pyrophosphoric acid , a polyphosphoric acid , apolymetaphosphoric acid salt, or an anhydrous phosphoric acid . Amongthese phosphoric acids, the non-condensed phosphoric acid isparticularly preferred.

The metal may preferably include a polyvalent metal, e.g., an alkalineearth metal, a transition metal, and metals of the groups 2B to 3B ofthe Periodic Table of Elements, particularly an alkaline earth metal.

As the metal phosphate (or metal salt of a phosphoric acid), there maybe mentioned a salt of the phosphoric acid with the polyvalent metal, inaddition a hydrogenphosphate corresponding to the polyvalent metalphosphate. The metal salt may be a double (or a triple) salt. Moreover,the metal salt may have a ligand.

As the metal phosphate, there may be used, for example, a pyrophosphate(such as Ca₂P₂O₇), a polymetaphosphate (such as Ca₃(P₃O₉)₂), a salt ofanhydrous phosphoric acid (such as Ca2(P₄O₁₂) or Ca₅(P₃O₁₀)₂), inaddition a condensed phosphate (such as Ca₅(PO₄)₃(OH) or Ca₅(PO₄)₃(F,Cl)), and there is preferably used a hydrogenphosphate.

Such a hydrogenphosphate may include, for example, a non-condensedhydrogenphosphate such as an alkaline earth metal hydrogenphosphate(e.g., a magnesium hydrogen orthophosphate, and a calcium hydrogenorthophosphate); a transition metal hydrogenphosphate (e.g., manganesehydrogenphosphate, and iron hydrogenphosphate); a hydrogenphosphate ofthe metal of the Group 2B of the Periodic Table of Elements (such aszinc hydrogenphosphate); a hydrogenphosphate of the metal of the Group3B of the Periodic Table of Elements (such as aluminumhydrogenphosphate); or a hydrogenphosphate of the metal of the Group 4Bof the Periodic Table of Elements [e.g., tin hydrogenphosphate (such astin dihydrogenphosphate or tin monohydrogenphosphate)]. Among them, asubstantially anhydrous metal hydrogenphosphate, particularly analkaline earth metal hydrogenphosphate [for example, magnesiumdihydrogenphosphate, calcium dihydrogenphosphate, calciummonohydrogenphosphate (calcium secondary phosphate (CaHPO₄)), bariumdihydrogenphosphate, and barium monohydrogenphosphate], is preferred.

(Metal Stannate)

Examples of the stannic acid may include stannic acid, metastannic acid,orthostannic acid, hexahydroxostannic acid, or others. As a metal, theremay be exemplified an alkali metal, and a polyvalent metal such as analkaline earth metal, a transition metal, or the metal of the Group 2Bof the Periodic Table of Elements. The metal stannate is usually ahydrous salt and includes, for example, an alkali metal stannate (e.g.,sodium stannate, and potassium stannate), an alkaline earth metalstannate (e.g., magnesium stannate), a transition metal stannate (e.g.,cobalt stannate), and a stannate of the metal of the Group 2B of thePeriodic Table of Elements (e.g., a (hydrous) zinc stannate). Amongthese metal stannates, a stannate of the metal of the Group 2B of thePeriodic Table of Elements, in particular a (hydrous) zinc stannate, ispreferred. These metal stannates may be used singly or in combination.

As a metal salt of an inorganic acid (oxygen acid) other than thephosphoric acid, the boric acid and the stannic acid, there may be usedvarious metal salts corresponding to the metal phosphate, the metalborate and the metal stannate.

(Metal Oxide, Metal Hydroxide and Metal Sulfide)

The metal in the metal oxide, the metal hydroxide, and the metal sulfidemay include an alkali metal (e.g., Li, Na, and K), an alkaline earthmetal (e.g., Mg, Ca, and Ba), and a metal of the group 4A (e.g., Ti, andZr), a metal of the group 5A (e.g., V), a metal of the group 6A (e.g.,Mo, and W), a metal of the group 7A (e.g., Mn), a metal of the group 8(e.g., Fe, Co, and Ni), a metal of the group 1B (e.g., Cu), a metal ofthe group 2B (e.g., Zn), a metal of the group 3B (e.g., Al), a metal ofthe group 4B (e.g., Sn) and a metal of the group 5B (e.g., Sb) of thePeriodic Table of Elements.

Examples of the metal oxide may include magnesium oxide, molybdenumoxide, tungstic oxide, titanium oxide, zirconium oxide, tin oxide,copper oxide, zinc oxide, aluminum oxide, nickel oxide, iron oxide,manganese oxide, antimony trioxide, antimony tetraoxide, and antimonypentaoxide.

The metal hydroxide may include, for example, aluminum hydroxide,magnesium hydroxide, tin hydroxide, and zirconium hydroxide.

The metal sulfide may include, for example, zinc sulfide, molybdenumsulfide, and tungsten sulfide. Among these metal sulfides, zinc sulfideis preferred. The metal oxides, the metal hydroxides, and the metalsulfides may be respectively used singly or in combination.

In the combinations of the base resin, the flame retardant (A) and theflame-retardant auxiliary (B), the preferred combination may include,for example, the following combinations (i), (ii), and others.

(i) base resin: a base resin at least comprising the aromaticpolyester-series resin,

flame retardant (A): a salt of at least one amino group-containingtriazine compound selected from the group consisting of melamine and thecondensate thereof (melam, melem and/or melon) with at least one memberselected from the group consisting of the sulfuric acid and the sulfonicacid, and

flame-retardant auxiliary (B): at least one member selected from thegroup consisting of (a) a salt of cyanuric acid with acetyleneurea, uricacid, melamine or the condensate thereof (melam, melem and/or melon),and (b) melamine or the condensate thereof (melam, melem and/or melon);

(ii) base resin: a base resin at least comprising the polyester-seriesresin (e.g., the PET, the PBT, a mixture of the PPT and the PET, or amixture of the PBT and the PET),

flame retardant (A): a salt of at least one aminotriazine compoundselected from the group consisting of melamine and the condensatethereof with at least one member selected from the group consisting ofthe sulfuric acid and the sulfonic acid (e.g., an alkanesulfonic acid),and

flame-retardant auxiliary (B): the aromatic resin (Bl) (e.g., thearomatic epoxy resin).

[Proportions of Flame Retardant and Flame-Retardant Auxiliary to beUsed]

In the flame-retardant resin composition of the present invention,combination use of the sulfate and/or sulfonate of the aminogroup-containing triazine compound, and the specific flame-retardantauxiliary can impart a high flame retardancy to a wide range of baseresins (e.g., a polyester-series resin) without use of ahalogen-containing flame retardant and/or an organicphosphorus-containing flame retardant. The proportion of the flameretardant (A) relative to the resin component comprising the base resinand the aromatic resin (B1) may be selected from the range of about 0.1to 300 parts by weight relative to 100 parts by weight of the resincomponent, and is usually not more than 200 parts by weight (e.g., about1 to 200 parts by weight), preferably about 3 to 150 parts by weight,and more preferably about 5 to 100 parts by weight, relative to 100parts by weight of the resin component.

The proportion of the flame retardant (A) may be about 0.1 to 120 partsby weight, preferably about 1 to 110 parts by weight (e.g., about 5 to100 parts by weight), and more preferably about 10 to 100 parts byweight (e.g., about 15 to 90 parts by weight), relative to 100 parts byweight of the base resin. Moreover, the proportion of theflame-retardant auxiliary (B) may be about 0.001 to 100 parts by weight(e.g., about 0.001 to 90 parts by weight), and preferably about 0.005 to80 parts by weight (e.g., about 0.01 to 70 parts by weight), relative to100 parts by weight of the base resin. The proportion of theflame-retardant auxiliary (B) may be usually about 0.001 to 10 parts byweight (e.g., about 0.001 to 8 parts by weight), and preferably about0.005 to 7 parts by weight (e.g., about 0.01 to 6 parts by weight),relative to 100 parts by weight of the base resin.

The base resin is usually different from the aromatic resin (B1). Insuch a case, the proportion (weight ratio) of the base resin relative tothe aromatic resin (B1) [the base resin/the aromatic resin] is about50/50 to 100/0 (e.g., about 50/50 to 99.99/0.01), preferably about 55/45to 100/0 (e.g., about 55/45 to 99.99/0.01), and more preferably about60/40 to 100/0 (e.g., about 60/40 to 99.95/0.05).

The proportion (weight ratio) of the flame retardant (A) relative to theflame-retardant auxiliary (B) [the flame retardant (A)/theflame-retardant auxiliary (B)] is about 99/1 to 1/99, preferably about98/2 to 2/98, and more preferably about 97/3 to 3/97. Moreover, theproportion (weight ratio) of the flame retardant (A) relative to theflame-retardant auxiliary (B) may be, for example, about 99.99/0.01 to1/99 (e.g., about 99.99/0.01 to 20/80), and preferably about 99.96/0.04to 10/90 (e.g., about 99.95/0.05 to 20/80). Incidentally, the proportion(weight ratio) of the flame retardant (A) relative to the aromatic resin(B1) may be, for example, about 99.99/0.01 to 20/80, preferably about99.95/0.05 to 30/70, and more preferably about 99.9/0.1 to 40/60.

It is preferred that the flame-retardant auxiliary (B) usually containsat least one selected from the cyclic urea-series compound or thederivative thereof (B2) and the amino group-containing triazine compound(B3), particularly, at least the component (B2). Incidentally, in thecase where the flame-retardant auxiliary (B) contains both the cyclicurea-series compound or the derivative thereof (B2) and the aminogroup-containing triazine compound (B3), the proportion of the aminogroup-containing triazine compound (B3) is about 1 to 200 parts byweight, preferably about 5 to 100 parts by weight, and more preferablyabout 5 to 50 parts by weight, relative to 100 parts by weight of thecyclic urea-series compound (B2).

Moreover, the proportion of the aromatic resin (B1) in theflame-retardant auxiliary (B) may be suitably selected from a range inwhich flame retardancy can be imparted to the resin, and is, forexample, about 0 to 500 parts by weight (e.g., about 0 to 400 parts byweight), preferably about 1 to 400 parts by weight (e.g., about 1 to 300parts by weight), and more preferably about 1 to 200 parts by weight(e.g., about 2 to 150 parts by weight), relative to 100 parts by weightof tha total amount of the cyclic urea-series compound or the derivativethereof (B2) and the amino group-containing triazine compound (B3).Moreover, the proportion of the inorganic metal-series compound (B4) isabout 0 to 300 parts by weight (e.g., about 5 to 200 parts by weight),and preferably about 10 to 150 parts by weight relative to 100 parts byweight of the total amount of the cyclic urea-series compound or thederivative thereof (B2) and the amino group-containing triazine compound(B3).

[Additive]

If necessary, the flame-retardant resin composition of the presentinvention may comprise a variety of additives (for example, otherflame-retardant, an antioxidant, a stabilizer, a dripping inhibitor, alubricant, and a plasticizer). These additives may be used singly or incombination. The total content of the additive(s) is about 0.01 to 50parts by weight, preferably about 0.1 to 30 parts by weight, and morepreferably about 1 to 20 parts by weight, relative to 100 parts byweight of the base resin.

(Other Flame Retardant)

Incidentally, the flame-retardant resin composition of the presentinvention may comprise, in order to further impart flame retardancy tothe composition, other flame retardant(s), for example, anitrogen-containing flame retardant, a sulfur-containing flameretardant, a silicon-containing flame retardant, an alcohol-based flameretardant, an intumescent-series (expansive) flame retardant (e.g., anexpansive graphite), and others.

The nitrogen-containing flame retardant may include a salt of an aminogroup-containing triazine compound exemplified in the paragraph of theabove-mentioned flame retardant (A), with an oxygen acid other than asulfuric acid and a sulfonic acid [for example, an oxygen acid nothaving a sulfur atom (sulfur-free oxygen acid), e.g., a nitric acid, achloric acid (e.g., chloric acid, chlorous acid, and hypochlorous acid),a boric acid (e.g., a non-condensed boric acid such as orthoboric acidor metaboric acid; and a condensed boric acid such as tetraboric acid orboric anhydride), antimonic acid, molybdic acid, tungstic acid, stannicacid, and silicic acid], and others.

The sulfur-containing flame retardant may include an organic sulfonicacid (for example, an alkanesulfonic acid, a perfluoroalkanesulfonicacid, an arylsulfonic acid, and a sulfonated polystyrene), sulfamicacid, an organic sulfamic acid, a salt of an organic sulfonic acid amide(e.g., an ammonium salt, an alkali metal salt, and an alkaline earthmetal salt), and others.

The silicon-containing flame retardant may include a(poly)organosiloxane, for example, a dialkylsiloxane (e.g.,dimethylsiloxane), an alkylarylsiloxane (e.g., phenylmethylsiloxane), adiarylsiloxane, and a monoorganosiloxane (for instance, apolydimethylsiloxane, a polyphenylmethylsiloxane); or a copolymer; orothers. Moreover, as the (poly)organosiloxane, there may be also used abranched organosiloxane [e.g., trade name “XC99-B5664” (manufactured byToshiba Silicone Co., Ltd.), trade names “X-40-9243”, “X-40-9244” and“X-40-9805” (manufactured by Shin-Etsu Chemical Co., Ltd.), compoundsdescribed in Japanese Patent Application Laid-Open No. 139964/1998(JP-10-139964A)], a modified (poly)organosiloxane (for example, amodified silicone) having substituent (s) such as epoxy group, hydroxylgroup, carboxyl group, amino group, and ether group in the end or mainchain of the molecule.

Examples of the alcohol-based flame retardant may include a polyhydricalcohol (e.g., pentaerythritol), an oligomeric polyhydric alcohol (e.g.,dipentaerythritol, and tripentaerythritol), an esterified polyhydricalcohol, a substituted alcohol, a cellulose compound (e.g., cellulose,hemicellulose, lignocellulose, pectocellulolse, and adipocellulose), anda saccharide compound (e.g., a monosaccharide, and a polysaccharide).

These other flame retardants may be used singly or in combination. Thecontent of other flame retardant may be, for example, selected withinthe range of about 0.01 to 50 parts by weight, preferably about 0.05 to30 parts by weight, and particularly about 0.1 to 20 parts by weight,relative to 100 parts by weight of the base resin.

(Antioxidant or Stabilizer)

Moreover, the flame retardant resin composition of the present inventionmay comprise an antioxidant and/or a stabilizer to maintain thermalstability of the composition for a long term. The antioxidant and thestabilizer may include, for example, a phenol-series (e.g., hinderedphenols), amine-series (e.g., hindered amines), phosphorous-series,sulfur-series, hydroquinone-series, or quinoline-series antioxidant (orstabilizer), an inorganic stabilizer, a compound having a functionalgroup reactive to an active hydrogen atom (a reactive stabilizer), andothers.

The phenol-series (phenolic) antioxidant may include, for example, aC₂₋₁₀alkylene glycol-bis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate];a di- or trioxyC₂₋₄alkyleneglycol-bis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate]; a C₃₋₈alkylenetriol-bis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate]; a C₄₋₈alkylenetetraol-tetrakis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate] such as apentaerythritol-tetrakis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate];and others.

The amine-series antioxidant may include a hindered amine, for example,a tri- or tetraC₁₋₃alkylpiperidine or a derivative thereof, a bis (tri-,tetra- or pentaC₁₋₃alkylpiperidine) C₂₋₂₀alkylenedicarboxylic acid ester[e.g., bis(2,2,6,6-tetramethyl-4-piperidyl)oxalate],1,2-bis(2,2,6,6-tetramethyl-4-piperidyloxy)ethane, phenylnaphthylamine,N,N′-diphenyl-1,4-phenylenediamine, andN-phenyl-N′-cyclohexyl-1,4-phenylenediamine.

The phosphorus-series (or phosphorus-containing) antioxidant (orstabilizer) may include, for example, triisodecyl phosphite,diphenylisodecyl phosphate, a bis- or tris(t-butylphenyl)phosphate,tris(2-cyclohexylphenyl)phosphate, a bis(C₁₋₉alkylaryl)pentaerythritoldiphosphite [e.g., bis(2,6-di-t-butyl-4-methylphenyl)pentaerythritoldiphosphite], a triphenyl phosphate-series stabilizer, adiphosphonite-series stabilizer, and others. The organicphosphorus-containing stabilizer usually has a t-butylpheyl group.

The hydroquinone-series antioxidant may include, for example,2,5-di-t-butylhydroquinone, and the quinoline-series antioxidant mayinclude, for example, 6-ethoxy-2,2,4-trimethyl-1,2-dihydroquinone. Thesulfur-series (or sulfur-containing) antioxidant may include, forexample, dilaurylthiodipropionate, distearylthiodiproionate, and others.

The inorganic stabilizer may include an inorganic metal ormineral-series stabilizer (e.g., a hydrotalcite, and a zeolite), and asalt of an alkali metal or alkaline earth metal with a carboxylic acid(e.g., a salt of a carbonic acid (a carbonate), and a salt with anorganic carboxylic acid). As the hydrotalcite, hydrotalcites recited inJapanese Patent Application Laid-Open No. 1241/1985 (JP-60-1241A) andJapanese Patent Application Laid-Open No. 59475/1997 (JP-9-59475A), suchas hydrotalcite compounds represented by the following formula areusable.

[M²⁺ _(1-x)M³⁺ _(x)(OH)₂]^(x+)[A^(n−) _(x/n).mH₂O]^(x−)

In the formula, M²⁺ represents Mg²⁺, Mn²⁺, Fe²⁺, Co²⁺, or any of otherdivalent metal ions; M³⁺ represents Al³⁺, Fe³⁺, Cr³⁺, or any of othertrivalent metal ions; A^(n−) represents CO₃ ²⁻, OH⁻, HPO₄ ²⁻, SO₄ ²⁻, orany of other n-valent anions (particularly, monovalent or divalentanion); x is 0<x<0.5; and m is 0≦m<1.

These inorganic stabilizers may be used singly or in combination.Incidentally, the hydrotalcite is available from Kyowa Chemical IndustryCo., Ltd. under the trade name “DHT-4A”, “DHT-4A-2”, or “Alcamizer”. Thezeolite is not particularly limited to a specific one, and for example,a zeolite recited in Japanese Patent Application Laid-Open No.62142/1995 (JP-7-62142A) may be employed. Incidentally, A-type zeoliteis available as “ZEOLAM-series (A-3, A-4, A-5)”, “ZEOSTAR-series(KA100P, NA-100P, CA-100P)” or others, X-type zeolite as “ZEOLAM-series(F-9)”, “ZEOSTAR-series (NX-100P)” or others, and Y-type zeolite as“HSZ-series (320NAA)” or others, from Tosoh Corp. or Nippon ChemicalIndustrial Co., Ltd.

The salt of the alkali metal or alkaline earth metal with the carboxylicacid may include, for example, a carbonate (e.g., magnesium carbonate,and (light/colloidal/heavy) calcium carbonate), a salt of an organiccarboxylic acid [for example, a salt of a fatty acid (e.g., lithiumacetate, sodium acetate, potassium acetate, magnesium acetate, calciumacetate, lithium stearate, sodium stearate, potassium stearate,magnesium stearate, calcium stearate, and calcium 12-hydroxystearate),and a salt of an aromatic carboxylic acid (e.g., lithiumbenzoate, sodiumbenzoate, potassium benzoate., magnesium benzoate, and calciumbenzoate)].

The reactive stabilizer may include a compound having a functional groupreactive to an active hydrogen atom. As the compound having a functionalgroup reactive to an active hydrogen atom, there may be exemplified acompound having at least one functional group selected from a cyclicether group, an acid anhydride group, an isocyanate group, an oxazolinegroup (or ring), an oxazine group (or ring), a carbodiimide group, andothers. These reactive stabilizers may be used singly or in combination.

Examples of the compound having a cyclic ether group may include acompound having an epoxy group or an oxetane group. The compound havingan epoxy group may include, for example, an alicyclic compound (e.g.,vinylcyclohexene dioxide); a glycidyl ester compound (e.g., glycidylversatate, glycidyl benzoate, and diglycidyl terephthalate); a glycidylether compound (e.g., hydroquinone diglycidyl ether, and bisphenol Aglycidyl ether); a glycidyl amine compound; an epoxy group-containingvinyl copolymer; an epoxidized polybutadiene; a copolymer of anepoxidized diene-series monomer and styrene; a triglycidyl isocyanurate;an epoxy-modified (or epoxy-containing) (poly)organosiloxane; andothers. The compound having an oxetane group may include, for example,an oxetanyl ester compound such as [1-ethyl(3-oxetanyl)]methyl stearate,[1-ethyl(3-oxetanyl)]methyl versatate, [1-ethyl(3-oxetanyl)]methylbenzoate, or di[1-ethyl(3-oxetanyl)]methyl (o-, m-, or p-)phthalate; anoxetanyl ether compound [for example, an alkyloxetanyl compound such asdi[1-ethyl(3-oxetanyl)]methyl ether, an aryloxetanyl compound such as3-ethyl-3-(phenoxymethyl)oxetane, an aralkyl oxetanyl ether compound, abisphenol-based oxetane resin such as bisphenol-Adi[1-ethyl(3-oxetanyl)]methyl ether, and a novolak oxetane resin]; anoxetane-modified (poly)organosiloxane; and an alkyloxetanyl methylderivative (for example, [1-methyl(3-oxetanyl)]methyl derivative) whichcorresponds to the above-mentioned derivative having an oxetanyl unit{for example, a [1-ethyl(3-oxetanyl)]methyl derivative).

The compound having an acid anhydride group may include, for example, anolefinic resin having a maleic anhydride group (e.g., an ethylene-maleicanhydride copolymer, and a maleic anhydride-modified polypropylene), andothers. Examples of the compound having an isocyanate group may includean aliphatic isocyanate such as hexamethylene diisocyanate, an alicyclicisocyanate such as isophorone diisocyanate, an aromatic isocyanate suchas diphenylmethane isocyanate, a modified product thereof (e.g., atrimer of isophorone diisocyanate), and others.

The compound having an oxazoline group may include, for example, abisoxazoline compound such as 2,2′-phenylenebis(2-oxazoline), and avinyl-series resin having an oxazoline group (e.g., avinyloxazoline-modified styrenic resin). The compound having an oxazinegroup may include, for example, a bisoxazine compound such as2,2′-bis(5,6-dihydro-4H-1,3-oxazine).

As the compound having a carbodiimide group, there may be mentioned, forexample, a polyarylcarbodiimide such as a poly(phenylcarbodiimide), apolyalkylarylcarbodiimide such as a poly(2-methyldiphenylcarbodiimide),and a poly[alkylenebis(alkyl or cycloalkylaryl)carbodiimide] such as apoly[4,4′-methylenebis(2,6-diethylphenyl)carbodiimide.

These antioxidants and/or stabilizers may be used singly or incombination. The each contents of the antioxidant and the stabilizer maybe, for example, selected from the range of about 0 to 10 parts byweight (e.g., about 0.01 to 10 parts by weight), preferably about 0.05to 8 parts by weight, and particularly about 0.1 to 5 parts by weight,respectively, relative to 100 parts by weight of the base resin.Moreover, the proportion of the antioxidant may be about 0 to 3 parts byweight (e.g., about 0.01 to 2 parts by weight), and preferably about0.01 to 1 part by weight, relative to 100 parts by weight of the baseresin. The proportion of the stabilizer may be about 0 to 10 parts byweight (e.g., about 0.01 to 8 parts by weight), and preferably about0.01 to 6 parts by weight, relative to 100 parts by weight of the baseresin.

To the flame-retardant resin composition of the present invention may beadded a dripping inhibitor such as a fluorine-containing resin. Thefluorine-containing resin may include a homo- or copolymer of afluorine-containing monomer, a copolymer of the fluorine-containingmonomer and a copolymerizable monomer (e.g., ethylene, and propylene);for example, a homopolymer such as a polytetrafluoroethylene, apolychlorotrifluoroethylene, or a polyvinylidene fluoride, and acopolymer such as a tetrafluoroethylene-hexafluoropropylene copolymer, atetrafluoroethylene-perfluoroalkylvinyl ether copolymer, or anethylene-tetrafluoroethylene copolymer. These fluorine-containing resinsmay be used singly or in combination.

The fluorine-containing resin may be used in the form of particles, andthe mean particle size may for example be about 10 to 5,000 μm,preferably about 100 to 1,000 μm, and more preferably about 100 to 700μm.

The content of the dripping inhibitor (e.g., the fluorine-containingresin) is, for example, about 0 to 5 parts by weight (e.g., about 0.01to 5 parts by weight), preferably about 0.1 to 3 parts by weight, andmore preferably about 0.1 to 2 parts by weight, relative to 100 parts byweight of the base resin.

The composition of the present invention may be further improved informability (or moldability) by further adding a lubricant and/or aplasticizer.

The lubricant may include (a) a long chain fatty acid or a derivativethereof, (b) a polyoxyalkylene glycol, (c) a silicone-series compound,(d) a wax, and others. These lubricants may be used singly or incombination.

(a) Long Chain Fatty Acid or Derivative Thereof

The long chain fatty acid may be a saturated fatty acid or anunsaturated fatty acid. Moreover, a long chain fatty acid in which apart of hydrogen atoms is replaced with substituent(s) such as hydroxylgroup(s) may be used. Such a long chain fatty acid may include amonovalent or divalent fatty acid having a carbon atom of not less than10, for example, a monovalent saturated fatty acid having a carbon atomof not less than 10 (e.g., a C₁₀₋₃₄saturated fatty acid such as capricacid, lauric acid, myristic acid, pentadecylic acid, palmitic acid,stearic acid, arachidic acid, behenic acid, or montanic acid), amonovalent unsaturated fatty acid having a carbon atom of not less than10 (e.g., a C₁₀₋₃₄unsaturated fatty acid such as oleic acid, linoleicacid, linolenic acid, arachidonic acid, or erucic acid), and a divalentfatty acid (a bibasic fatty acid) having a carbon atom of not less than10 (e.g., a divalent C₁₀₋₃₀saturated fatty acid such as sebacic acid,dodecanoic diacid, tetradecanoic diacid, or thapsic acid; and a divalentC₁₀₋₃₀unsaturated fatty acid such as decenoic diacid, or dodecenoicdiacid). The fatty acid may also include a fatty acid having one or aplurality of hydroxyl group(s) in a molecule thereof (e.g., ahydroxy-saturated C₁₀₋₂₆fatty acid such as 12-hydroxystearic acid).Among these fatty acids, a monovalent C₁₀₋₂₆saturated or unsaturatedfatty acid, and a divalent C₁₀₋₂₀saturated or unsaturated fatty acid arepreferred.

The derivative of the long chain fatty acid may include a fatty acidester and a fatty acid amide, and others. The structure of the fattyacid ester is not particularly limited to a specific one, the fatty acidester may be either a linear or a branched one. Examples of the fattyacid ester may include an ester of a long chain fatty acid with analcohol (e.g., an ester having one or a plurality of ester bond(s), suchas a mono- to triester). The alcohol constituting the long chain fattyacid ester may be a monohydric alcohol, and usually, preferably apolyhydric alcohol.

The polyhydric alcohol may include a polyhydric alcohol having a carbonatom of about 2 to 8 and preferably of about 2 to 6, or a polymerthereof, for example, a diol such as an alkylene glycol (e.g., ethyleneglycol, diethylene glycol, and propylene glycol); a triol such asglycerin, trimethylolpropane, or a derivative thereof; a tetraol such aspentaerythritol, sorbitan, or a derivative thereof; and a homo- orcopolymer of such a polyhydric alcohol (e.g., a homo- or copolymer of apolyoxyalkylene glycol such as a polyethylene glycol or a polypropyleneglycol, and a polyglycerin). The average degree of polymerization of thepolyoxyalkylene glycol is not less than 2 (e.g., about 2 to 500),preferably about 2 to 400 (e.g., about 2 to 300), and more preferablynot less than 16 (e.g., about 20 to 200). Incidentally, in the case ofusing the polyoxyalkylene glycol as the polyhydric alcohol, it ispreferred to use, as the long chain fatty acid constituting the ester, afatty acid having a carbon atom of not less than 12, e.g., a monovalentC₁₂₋₂₆saturated or unsaturated fatty acid, and a divalentC₁₂₋₂₀saturated or unsaturated fatty acid.

Examples of such a fatty acid ester may include ethylene glycoldistearate, glycerin monostearate, glycerin tripalmitate, a polyglycerintristearate, trimethylolpropane monopalmitate, pentaerythritolmonoundecylate, sorbitan monostearate; and a monolaurate, monopalmitate,monostearate, dilaurate, dipalmitate, distearate, dibehenate,dimontanate, dioleate and dilinoleate of a polyalkylene glycol (e.g., apolyethylene glycol, and a polypropylene glycol).

Among the derivatives, as the fatty acid amide, an acid amide (e.g., amonoamide, and a bisamide) of the long chain fatty acid (the monovalentor divalent long chain fatty acid) with an amine (e.g., a monoamine, adiamine, and a polyamine) may be used. Among the acid amides, thebisamide is particularly preferred.

The monoamide may include, for example, a primary acid amide of asaturated fatty acid, such as capric acid amide, lauric acid amide,myristic acid amide, palmitic acid amide, stearic acid amide, arachidicacid amide, or behenic acid amide; a primary acid amide of anunsaturated fatty acid, such as oleic acid amide; a secondary acid amideof a saturated and/or unsaturated fatty acid with a monoamine, such asstearylstearic acid amide, or stearyloleic acid amide; and others.

Examples of the bisamide may include a bisamide of a C₁₋₆alkylenediamine(particularly, a C₁₋₂alkylenediamine) with the above-mentioned fattyacid, for example, ethylenediamine-distearic acid amide (e.g.,ethylenebisstearyl amide), hexamethylenediamine-distearic acid amide,ethylenediamine-dioleic acid amide, ethylenediamine-dierucic acid amide,and others. Moreover, as the bisamide, a bisamide in which differentacyl groups bond to an amine site of the alkylenediamine, such asethylenediamine- (stearic acid amide) oleic acid amide, may be alsoused.

(b) Polyoxyalkylene Glycol

The polyoxyalkylene glycol may include a homo- or copolymer of analkylene glycol [for example, a C₂₋₆alkylene glycol such as ethyleneglycol, propylene glycol, or tetramethylene glycol (preferably aC₂₋₄alkylene glycol)], a derivative thereof, and others.

The concrete examples of the polyoxyalkylene glycol may include apolyC₂₋₆oxyalkylene glycol such as a polyethylene glycol, apolypropylene glycol, or a polytetramethylene glycol (preferably apolyC₂₋₄oxyalkylene glycol), a polyoxyethylene-polyoxypropylenecopolymer (e.g., a random or block copolymer), a polyoxyethylenepolyoxypropylene glyceryl ether, and a polyoxyethylene polyoxypropylenemonobutyl ether.

(c) Silicone-Series Compound

The silicone-series compound may include a (poly)organosiloxane. The(poly)organosiloxane may include a monoorganosiloxane such as adialkylsiloxane (e.g., dimethylsiloxane), an alkylarylsiloxane (e.g.,phenylmethylsiloxane), or a diarylsiloxane (e.g., diphenylsiloxane), ahomopolymer thereof (e.g., a polydimethylsiloxane, and apolyphenylmethylsiloxane) or a copolymer thereof. Moreover, the(poly)organosiloxane may include a modified (poly)organosiloxane (e.g.,a modified silicone) having a substituent (such as epoxy group, hydroxylgroup, carboxyl group, amino group or ether group) at a terminal or amain chain in a molecule thereof.

(d) Wax

The wax may include a natural paraffin, a synthetic paraffin, a microwax, a polyolefinic wax, and others. The polyolefinic wax may include apolyC₂₋₄olefinic wax such as a polyethylene wax or a polypropylene wax,an olefin copolymer wax such as an ethylene copolymer wax, and others,and may also include a partially oxidized matter thereof or a mixturethereof.

The olefin copolymer wax may include, for example, a copolymer of anolefin (e.g., an a-olefin such as ethylene, propylene, 1-butene,2-butene, isobutene, 3-methyl-1-butene, 4-methyl-1-butene,2-methyl-2-butene, 4-methyl-1-pentene, 1-hexene, 2,3-dimethyl-2-butene,1-heptene, 1-octene, 1-nonene, 1-decene, or 1-dodecene), and a copolymerof such an olefin and a copolymerizable monomer. Examples of thecopolymerizable monomer may include a polymerizable monomer such as anunsaturated carboxylic acid or an acid anhydride thereof [e.g., maleicanhydride, and (meth)acrylic acid], or a (meth)acrylic acid ester [e.g.,a C₁₋₁₀alkyl(meth)acrylate such as methyl(meth)acrylate,ethyl(meth)acrylate, propyl(meth)acrylate, butyl(meth)acrylate, or2-ethylhexyl(meth)acrylate (preferably a C₁₋₄alkyl(meth)acrylate)].Incidentally, these copolymers may be a random copolymer, a blockcopolymer, and a graft copolymer. As the olefin copolymer wax, acopolymer of ethylene and at least one monomer selected from the groupconsisting of other olefin and a polymerizable monomer is preferred.

Moreover, the content of the lubricant may be about 0 to 2 parts byweight (about 0.01 to 2 parts by weight), and preferably about 0.05 to1.5 parts by weight, relative to 100 parts by weight of the base resin.

The plasticizer may include a polyester-series compound [e.g.,(di)ethylene glycol dibenzoate, 2-methyl-1,3-dihydroxypropanedibenzoate, neopentyl glycol dibenzoate, a polyethylene glycolmono-ordibenzoate, a polycaprolactone mono- or dibenzoate; and a long chainfatty acid ester of a C₁₋₃alkylene oxide (e.g., ethylene oxide, andpropylene oxide) adduct of a biphenol or bisphenol compound (e.g.,bisphenol A)], an adipic acid ester compound (e.g. ,di-2-ethylhexyladipate), a citric acid ester-series compound, a phthalicacid ester-series compound (e.g., di-2-ethylhexyl phthalate), atetrahydrophthalic acid ester-series compound, a trimellitic acidester-series compound (e.g., tri-2-ethylhexyl trimellitate), anether-series compound [e.g., a C₁₋₃alkylene oxide (e.g., ethyleneoxideand propyleneoxide) adduct of a biphenol or bisphenol compound (e.g.,bisphenol A)], a phosphoric ester-series compound (e.g., an alkyl estersuch as trimethyl phosphate; an aryl ester such as tricresyl phosphate,or cresyl diphenyl phosphate; and a bisphenol-series aromatic condensedphorphoric ester). These plasticizers may be used singly or incombination.

The content of the plasticizer is, for example, about 0 to 20 parts byweight (e.g., about 0.01 to 20 parts by weight), and preferably about 0to 10 parts by weight (e.g., about 0.01 to 10 parts by weight), relativeto 100 parts by weight of the base resin.

Further, the flame-retardant resin composition of the present inventionmay contain other additive(s), for example, a stabilizer (e.g., anultraviolet ray absorbing agent, a heat stabilizer, and aweather-resistant stabilizer), a mold-release-agent (releasing agent), acoloring agent, an impact resistance improver (impact modifier), a slip-(friction/wear) improving agent, and others.

[Filler]

The flame-retardant resin composition of the present invention may bemodified with the use of a filler [for example, a fibrous filler, and anon-fibrous filler (such as a plate-like one or a particulate one)]tofurther improve mechanical strength, rigidity, thermal stability,electrical property and others.

As the fibrous filler, there may be mentioned a glass fiber, an asbestosfiber, a carbon fiber, a silica fiber, a silica-alumina fiber, azirconia fiber, a potassium titanate fiber, a metal fiber, and anorganic fiber having high melting point.

Among the non-fibrous fillers, the plate-like filler may include, forexample, a glass flake, a mica, a graphite, a variety of metal foil, andothers. The particulate filler includes a carbon black, a silica, apowder of quartz, a glass bead, a glass powder, a milled fiber, asilicate [e.g., a calcium silicate, an aluminum silicate, a kaolin, atalc, a mica, a clay, a diatomite, and a wollastonite], a metalcarbonate (e.g., a calcium carbonate, and a magnesium carbonate), ametal sulfate (e.g., a calcium sulfate, and a barium sulfate), and ametal powder such as a silicon carbide. The preferred filler may includea fibrous filler (e.g., a glass fiber, and a carbon fiber), anon-fibrous filler (e.g., a particulate or plate-like filler, inparticular a glass bead, a mild fiber, a kaolin, a talc, a mica, and aglass flake). The particularly preferred filler may include a glassfiller, e.g., a glass fiber (e.g., chopped strand).

The proportion of the filler in the flame-retardant resin compositionis, for example, about 1 to 60% by weight, preferably about 1 to 50% byweight, and more preferably about 1 to 45% by weight. The proportion ofthe filler may be, for example, about 0 to 100 parts by weight (e.g.,about 0.1 to 100 parts by weight), preferably about 10 to 100 parts byweight (e.g., about 30 to 90 parts by weight), and more preferably about35 to 80 parts by weight, relative to 100 parts by weight of the baseresin. Moreover, the proportion of the filler may be about 0 to 30 partsby weight (e.g., about 0.01 to 30 parts by weight), and preferably about0.1 to 25 parts by weight.

If necessary, the filler may be treated with a sizing agent orsurface-treatment agent (e.g., a functional compound such as anepoxy-series compound, silane-series compound, or a titanate-seriescompound, preferably an epoxy-series compound such as a bisphenolA-based epoxy resin, or a novolak epoxy resin). The time to treat thefiller may be the same time with addition thereof, or the time precedentto addition thereof. Moreover, the amount of the functionalsurface-treatment agent or sizing agent to be used is about not morethan 5% by weight, and preferably about 0.05 to 2% by weight relative tothe filler.

The resin composition of the present invention may comprise at least onemember selected from the group constituting of the antioxidant, thestabilizer, the dripping inhibitor, the lubricant, the plasticizer, andthe filler, in addition to the above-mentioned essential components (thebase resin, the flame retardant (A) and the flame-retardant auxiliary(B1)).

The flame-retardant resin composition of the present invention may be aparticulate mixture or a molten mixture, and it may be prepared bymixing (or melt-kneading) the base resin with the flame retardant, theflame-retardant auxiliary, and if necessary, the dripping inhibitor orother additive(s) in a conventional manner. The flame-retardant resincomposition may be in the form of a pellet. Incidentally, as aproduction process of pellets with an extruder, for example, thefollowing process is available: a production process comprisingprecedently melt-mixing all components except for a brittle or fragilefiller (such as a glass-series filler), and then mixing the brittle orfragile filler with the mixture.

Incidentally, for imparting handling, it is usable the master batchprepared by melt-mixing a non-resinous component(s) and a resinouscomponent(s). The flame-retardant resin composition can be produced bymelt-mixing the master batch, the base resin, and if necessary theresidual component(s).

Moreover, the flame-retardant resin composition may be produced bymixing the base resin, the flame retardant (A), and the flame-retardantauxiliary (B).

The present invention also ensures improvement in the electricalproperty (e.g., tracking resistance) of the shaped article. Therefore,the present invention also includes a method for improving (orenhancing) at least one property selected from the group consisting offlame retardancy, bleed out resistance and electrical properties (e.g.,tracking resistance).

The shaped article (molded article, shaped member) of the presentinvention may be formed from the flame-retardant resin composition.

The shaped article of the present invention has both flame retardancyand electrical property. That is, the shaped article may have acomparative tracking index of not less than 300 V (e.g., about 300 to1000 V), preferably not less than 350 V (e.g., about 350 to 900 V), andmore preferably about 400 to 800 V as the electrical property. Moreover,the shaped article may have a flame-retardant performance of V-2, V-1 orV-0 in a flame retardancy test measured by using a test piece having athickness of 0.8 mm in accordance with UL94 as the flame retardancy.

The present invention also includes a process for producing a shapedarticle which comprises injection molding a flame-retardant resincomposition comprising the base resin, the flame retardant (A), and theflame-retardant auxiliary (B).

INDUSTRIAL APPLICABILITY

The flame-retardant resin composition of the present invention can bemelt-kneaded and shaped or molded by a conventional method such asextrusion molding, injection molding, or compression molding, and isexcellent in flame retardancy and molding processability, and the resincomposition (thus formed shaped article) may be utilized for variouspurposes. For example, the shaped article is suitable for an electricand/or electronic device part, a household electrical appliance part, anoffice automation (OA) device part, a mechanical device part, anautomotive part, a packaging material or a case, and others. Moreover,the shaped article of the present invention is concretely usable for aconnector part, a switch part, a relay part, a transformer part, abreaker part, an electromagnetic switch device part, a focus case part,a capacitor part, a motor part, a copying machine part, a printer part,and others.

EXAMPLES

The following examples are intended to describe this invention infurther detail and should by no means be interpreted as defining thescope of the invention.

Incidentally, flame retardancy and blooming properties of a resincomposition were evaluated on the basis of the following tests.

(Evaluation of Flame Retardancy)

In accordance with UL94, the flame retardancy was evaluated using a testpiece 3.2 mm thick (Examples 1 to 15 and Comparative Examples 1 to 8).Incidentally, in Examples 16 to 34 and Comparative Examples 9 to 17, theflame retardancy based on UL94 was evaluated using a test piece 0.8 mmthick.

(Evaluation of Blooming Properties)

A test piece 1.6 mm thick for burning was heated at 150° C. for 5 hours,and visually observed for the state of bleeding out in the surface ofthe test piece. The blooming properties were evaluated on the basis ofthe following judgmental standard.

“A”: no bleeding out was observed

“B”: slight bleeding out was observed

“C”: remarkable bleeding out was observed

(Tracking Resistance)

In accordance with IEC112 standard, comparative tracking index (V) wasmeasured by using a flat plate (70 mm×50 mm×3 mm), and electricalproperty (or insulating property) was evaluated.

Moreover, components used in Examples and Comparative Examples are shownas follows.

[Base Resin R]

R-1: Polybutylene terephthalate [“DURANEX”, intrinsic viscosity=1.0,manufactured by Polyplastics Co., Ltd.]

R-2: Polyethylene terephthalate [“BELLPET EFG 10”, manufactured byKanebo, Ltd.]

R-3: Acrylonitrile-styrene copolymer [“CEVIAN N JD”, manufactured byDaicel Chemical Industries, Ltd.]

R-4: Polypropylene terephthalate [prepared by polycondensation ofdimethyl terephthalate and 1,3-propanediol; intrinsic viscosity=1.0]

[Flame retardant (salt of amino group-containing triazine compound withsulfuric acid or sulfonic acid) A]

A-1: Melamine sulfate [a material obtained by heat-treating “APINON-901”(manufacture by Sanwa Chemical Co., Ltd.) at 200° C. for 2 hours under anitrogen flow: incidentally, the heat-treated material had a thermalweight decrease of not larger than 1% by weight by thermogravimetry whenthe material was heated with increasing a temperature from 30° C. to250° C. at a ΔT of 20° C./minute under a nitrogen flow by using acalorimetric analysis apparatus (Perkin-Elmer TGA-7)]

A-2: Melam methanesulfonate [“MMS-200”, manufactured by Nissan ChemicalIndustries, Ltd.]

Compound Used in Comparative Examples

A-3: Resorcinol bis(diphenyl phosphate) [“REOFOS RDP”, manufactured byAjinomoto-Fine-Techno Co., Inc.]

A-4: Melamine sulfate [“APINON-901”, manufacture by Sanwa Chemical Co.,Ltd., which had a thermal weight decrease of 9.1% by weight bythermogravimetry]

[Flame-Retardant Auxiliary B]

[Aromatic Resin (B1)]

B1-1: Novolak phenol resin [dimerless phenol-novolak resin, “PR-53647”,manufactured by Sumitomo Durez Co., Ltd]

B1-2: Glycidylated novolak resin [“EPPN”, manufactured by Nippon KayakuCo., Ltd.]

B1-3: Bisphenol A-based epoxy resin [“EPIKOTE 1004K”, manufactured byYuka Shell Epoxy K.K.]

[Cyclic urea-series compound or derivative thereof (B2)]

B2-1: Melamine cyanurate [“MC610”, manufactured by Nissan ChemicalIndustries, Ltd.]

B2-2: Acetyleneurea [manufactured by Tokyo Kasei Kogyo Co., Ltd.]

[Amino Group-Containing Triazine Compound (B3)]

B3-1: Melem [manufactured by Nissan Chemical Industries, Ltd.]

[Inorganic Flame Retardant (B4)]

B4-1: Zinc borate [“FireBrake ZB”, manufactured by Borax Japan Ltd.]

B4-2: Anhydrous dibasic calcium phosphate: mean particle size=about 30μm [manufactured by Taihei Chemical Industrial Co., Ltd.]

[Antioxidant C]

Pentaerythritol tetrakis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate][“IRGANOX 1010”, manufactured by Ciba-Geigy Ltd]

[Stabilizer D]

[Phosphorus-Series Stabilizer D1]

D1-1: Tetrakis(2,4-di-t-butylphenyl)-4,4′-biphenylene diphosphonite[“SANDOSTAB P-EPQ”, manufactured by Sandoz.]

D1-2:

Bis(2,6-di-t-butyl-4-methylphenyl)pentaerythritol diphosphite [“ADKSTABPEP36”, manufactured by Adeka Argus Chemical Co., Ltd.]

D1-3: Sodium dihydrogenphosphate dihydrate

[Reactive Stabilizer D2]

D2-1: Glycidyl benzoate

D2-2: Glycidyl versatate

[Inorganic Stabilizer D3]

D3-1: Sodium stearate

D3-2: Calcium carbonate

[Dripping Inhibitor E]

Polytetrafluoroethylene

[Lubricant F]

F-1: Montanic acid ester [“LICOLUB WE4”, manufactured by Clariant Ltd.]

F-2: Montanic acid ester [“LUZA WAX-P”, manufactured by Toyo-PetroliteCo., Ltd.]

[Plasticizer G]

G-1: Tri-2-ethylhexyltrimellitate [TOTM”, manufactured by DaihachiChemical Industry Co., Ltd.]

G-2: Polycaprolactone dibenzoate [“PLACCEL”, manufactured by DaicelChemical Industries, Ltd.]

G-3: Polydimethylsiloxane [“TORAYFIL”, manufactured by Dow Corning ToraySilicone Co., Ltd.]

[Filler H]

Glass-chopped strand being 10 μm in diameter and 3 mm long

Examples 1 to 15 and Comparative Examples 1 to 8

The above components were mixed in the ratio (parts by weight) describedin Tables 1 and 2, and the mixture was kneaded with the use of a smallextruder [“Laboplastmill 4C150” manufactured by Toyo Seiki Seisaku-sho,Ltd.] to prepare a resin composition. The obtained resin composition wassubjected to injection molding by an injection molding machine to makeshaped articles for test. The properties were evaluated with the use ofthe test shaped articles. The results are shown in Tables 1 and 2.

Examples 16 to 35, and Comparative Examples 9 to 17

The components shown in Tables 3 and 4 were mixed in the ratio (parts byweight) described in Tables 3 and 4, and the mixture was extruded by a30 mmφ biaxial extruder [“TEX30” manufactured by Japan Steel Works,Ltd.] to prepare a resin composition. The resin composition wassubjected to injection molding by an injection molding machine to makeshaped articles for test. The properties were evaluated with the use ofthe test shaped articles. The results are shown in Tables 3 and 4.

TABLE 1 Examples 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 Base resin R R-1 5050 50 50 50 50 50 50 50 — — — — — — R-2 50 50 50 50 50 50 50 50 50 100100 100 100 100 90 R-3 — — — — — — — — — — — — — — 10 Flame retardant AA-1 A-1 A-1 A-1 A-2 A-1 A-1 A-1 A-1 A-1 A-1 A-1 A-2 A-1 A-1 40 40 40 4040 40 40 40 40 40 40 40 40 40 40 Flame-retardant B2 B2-1 B2-1 B2-1 B2-1B2-1 B2-1 B2-1 B2-1 B2-1 B2-1 B2-1 B2-1 B2-1 B2-1 B2-1 auxiliary B 40 4040 40 40 35 35 40 40 40 40 40 40 35 40 B2-2 B2-2 5 5 B1- B1-1 B1-2 B1-3— — — B3-1 B4-1 B4-2 B1-3 — — — — — B3 15 5 3 5 15 25 3 Antioxidant C0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 Stabilizer DD1 D1-1 D1-1 — D1-2 D1-2 D1-3 D1-2 D1-2 D1-2 — D1-2 D1-1 D1-2 D1-1 D1-20.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 D2 — — D2-1 — — — —— — D2-2 — — — — — 1.0 1.0 D3 — — D3-1 — — — — — — D3-1 — — — — — 0.050.05 Dripping inhibitor E 1.3 1.3 1.3 1.3 1.3 1.3 1.3 1.3 1.3 1.3 1.31.3 1.3 1.3 1.3 Lubricant F F-1 0.7 0.7 0.7 — — — — — — 0.7 — — — — —F-2 — — — 0.7 0.7 0.7 0.7 0.7 0.7 — 0.7 0.7 0.7 0.7 0.7 Plasticizer G —— — — — — — — — — — G-1 — G-2 G-3 5 5 5 Filler H 65 80 80 80 80 80 80 6550 80 80 80 80 80 80 UL94 Flame V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0V-0 V-0 V-0 V-0 V-0 retardancy Blooming property A A A A A A A A A A A AA A A

TABLE 2 Comparative Examples 1 2 3 4 5 6 7 8 Base resin R R-1 50 50 5050 — — — — R-2 50 50 50 50 100 100 100 100 Flame retardant A A-1 — 40 —— — 40 — — A-3 — — — 40 — — — 40 Flame-retardant — — B2-1 B2-1 — — B2-1B2-1 auxiliary B 40 40 40 40 Antioxidant C 0.7 0.7 0.7 0.7 0.7 0.7 0.70.7 Stabilizer D D1-2 D1-2 D1-2 D1-2 D1-2 D1-2 D1-2 D1-2 0.5 0.5 0.5 0.50.5 0.5 0.5 0.5 Dripping inhibitor E 1.3 1.3 1.3 — 1.3 1.3 1.3 —Lubricant F F-2 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 Plasticizer G — — — — —— — — Filler H 80 80 80 80 80 80 80 80 UL94 Flame HB HB HB V-2 HB HB HBV-2 retardancy Blooming property A A A B A A A B

TABLE 3 Examples 16 17 18 19 20 21 22 23 24 25 26 27 28 29 Base resin RR-1 100 100 80 70 50 50 60 50 50 50 50 50 50 50 R-2 — — 20 30 50 50 4050 50 50 50 50 50 50 R-3 — — — — — — — — — — — — — — R-4 — — — — — — — —— — — — — — Flame retardant A A-1 A-1 A-2 A-1 A-1 A-1 A-1 A-1 A-1 A-1A-1 A-1 A-1 A-1 15 25 25 100 85 85 85 80 85 85 85 85 80 80Flame-retardant B1-2 B1-3 B1-3 B1-3 B1-1 B1-2 B1-3 B1-3 B2-1 B2-2 B3-1B4-1 B1-3 B1-3 auxiliary B 0.5 0.5 0.5 1.0 0.5 2.5 2.5 5.0 2.5 2.5 2.52.5 2.5 2.5 B2-1 B4-1 2.5 2.5 Antioxidant C 0.5 0.5 0.5 0.5 0.5 0.5 0.50.5 0.5 0.5 0.5 0.5 0.5 0.5 Stabilizer D D-1 — — D1-1 D1-2 D1-1 D1-1D1-1 D1-1 D1-1 D1-1 D1-1 D1-1 D1-1 D1-1 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.50.5 0.5 0.5 0.5 D-2 — — — — — — — — — — — — — — D-3 — — — — — — — — — —— — — — Dripping inhibitor E — — — 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.01.0 1.0 Lubricant F F-1 — — — 0.7 — — — — — — — — — — F-2 — — — — 0.70.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 Plasticizer G — — — — — — — — — — —— — — Filler H — — — 50 60 60 60 45 60 60 60 60 60 60 UL94 Flame V-2 V-2V-2 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 retardancy Bloomingproperty A A A A A A A A A A A A A A Comparative >600 >600 >600 450 450450 450 500 450 450 450 450 450 450 tracking index (V)

TABLE 4 Examples Comparative Examples 30 31 32 33 34 35 9 10 11 12 13 1415 16 17 Base resin R R-1 50 50 50 — — — 100 100 50 60 50 50 50 50 50R-2 50 50 50 100 100 50 — — 50 40 50 50 50 50 50 R-3 — — — — — — — — — —— — — — — R-4 — — — — — 50 — — — — — — — — — Flame retardant A A-1 A-2A-4 A-1 A-1 A-1 — — — — — — — — — 85 85 85 75 85 85 Flame-retardant B1-3B1-3 B1-3 B1-3 B1-3 B1-3 — B1-2 — B1-1 B1-2 B1-3 B2-1 B3-1 B4-1auxiliary B 2.5 5.0 2.5 2.5 5.0 2.5 0.5 2.5 2.5 2.5 2.5 2.5 2.5Antioxidant C 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.50.5 Stabilizer D D-1 D1-1 D1-1 D1-1 D1-1 D1-2 D1-1 — — — — — — — — — 0.50.5 0.5 0.5 0.5 0.5 D-2 D2-2 — — — — — — — — — — — — — — 1.5 D-3 2.5 — —— — — — — — — — — — — — Dripping inhibitor E 1.0 1.0 1.0 1.0 1.0 1.0 — —— — — — — — — Lubricant F F-1 — — — — — — — — — — — — — — F-2 0.7 0.70.7 0.7 0.7 0.7 — — 0.7 0.7 0.7 0.7 0.7 0.7 0.7 Plasticizer G — — — —G-2 — — — — — — — — — — 5.0 Filler H 60 60 60 60 50 60 — — 60 60 60 6060 60 60 UL94 Flame V-0 V-0 V-1 V-0 V-0 V-0 HB HB HB HB HB HB HB HB HBretardancy Blooming property A A A A A A A A A A A A A A A Comparative450 450 400 400 400 450 >600 >600 >600 >600 >600 >600 >600 >600 >600tracking index (V)

1. A flame-retardant resin composition, which comprises (R) a baseresin, (A) a flame retardant and (B) a flame-retardant auxiliary,wherein the flame retardant (A) comprises a salt of (A1) an aminogroup-containing triazine compound with (A2) at least one memberselected from the group consisting of a sulfuric acid and a sulfonicacid, and the flame-retardant auxiliary (B) comprises at least onemember selected from the group consisting of (B1) an aromatic resin,(B2) a cyclic urea-series compound or a derivative thereof, (B3) anamino group-containing triazine compound and (B4) at least one inorganicmetal-series compound selected from the group consisting of metalborates, metal hydrogen phosphates, metal stannates, metal molybdates,metal tungstates and metal sulfides.
 2. A resin composition according toclaim 1, wherein the base resin (R) comprises (i) a polyester-seriesresin, or (ii) a polyester-series resin and a polystyrenic resin.
 3. Aresin composition according to claim 1, wherein the base resin (R)comprises a homo- or copolyester having at least one unit selected fromthe group consisting of 1,4-cyclohexanedimethylene terephthalate, aC₂₋₄alkylene terephthalate, and a C₂₋₄alkylene naphthalate.
 4. A resincomposition according to claim 1, wherein the base resin (R) comprisesat least one member selected from the group consisting of a polyethyleneterephthalate, a polypropylene terephthalate, a polybutyleneterephthalate, and an isophthalic acid-modified polybutyleneterephthalate.
 5. A resin composition according to claim 1, wherein thebase resin (R) comprises a mixture of a first resin and a second resin,the first resin is selected from the group consisting of apolyC₃₋₄alkylene terephthalate, the second resin is a polyethyleneterephthalate or a polybutylene terephthalate and is different from thefirst resin, and the mixture is (i) a mixture of a polybutyleneterephthalate and a polyethylene terephthalate, (ii) a mixture of apolypropylene terephthalate and a polyethylene terephthalate, or (iii) amixture of a polypropylene terephthalate and a polybutyleneterephthalate.
 6. A resin composition according to claim 1, wherein thebase resin (R) is a mixture of a polybutylene terephthalate and apolyethylene terephthalate, or a mixture of a polypropyleneterephthalate and a polyethylene terephthalate.
 7. A resin compositionaccording to claim 5, wherein the proportion of the first resin relativeto the second resin [the first resin/the second resin] is 20/80 to 80/20in a weight ratio.
 8. A resin composition according to claim 1, whereinthe amino group-containing triazine compound (Al) in the flame retardant(A) comprises melamine or a melamine condensate.
 9. A resin compositionaccording to claim 1, wherein the proportion of the aminogroup-containing triazine compound (A1) relative to the total amount ofthe sulfuric acid and the sulfonic acid (A2) in the flame retardant (A)is 1/5 to 5/1 in a molar ratio.
 10. A resin composition according toclaim 1, wherein the salt of the amino group-containing triazinecompound with at least one member selected from the group consisting ofthe sulfuric acid and the sulfonic acid has a weight decrease of notlarger than 15% by weight when the salt is heated with increasing atemperature from 30 to 250° C. at an increasing rate of 20° C. perminute under a nitrogen flow.
 11. A resin composition according to claim1, wherein the aromatic resin (B1) comprises at least one memberselected from the group consisting of a resin containing an aromaticring having a hydroxyl group and/or an amino group, a polyarylate-seriesresin, an aromatic epoxy resin, an aromatic nylon, a polyphenylenesulfide-series resin, a polyphenylene oxide-series resin, and apolycarbonate-series resin.
 12. A resin composition according to claim1, wherein the cyclic urea-series compound or a derivative thereof (B2)comprises at least one member selected from the group consisting of acyclic ureide, and a salt of a cyclic ureide with a melamine.
 13. Aresin composition according to claim 1, wherein the aminogroup-containing triazine compound (B3) comprises at least one memberselected from the group consisting of melamine or a derivative thereofand guanamine or a derivative thereof.
 14. A resin composition accordingto claim 1, wherein the inorganic metal-series compound (B4) comprisesat least one member selected from the group consisting of a metal saltof an oxygen acid having no sulfur atom, a metal oxide, a metalhydroxide and a metal sulfide.
 15. A resin composition according toclaim 1, wherein the proportion of the flame retardant (A) relative tothe flame-retardant auxiliary (B) is 99.99/0.01 to 1/99 in a weightratio.
 16. A resin composition according to claim 1, wherein the baseresin (R) comprises at least a polyester-series resin, the flameretardant (A) comprises a salt of at least one amino group-containingtriazine compound selected from the group consisting of melamine and acondensate thereof with at least one member selected from the groupconsisting of the sulfuric acid and the sulfonic acid, and theflame-retardant auxiliary (B) comprises the aromatic resin (B1).
 17. Aresin composition according to claim 1, wherein the base resin (R)comprises at least (i) a polyethylene terephthalate, (ii) a polybutyleneterephthalate, (iii) a mixture of a polypropylene terephthalate and apolyethylene terephthalate, or (iv) a mixture of a polybutyleneterephthalate and a polyethylene terephthalate, the flame retardant (A)comprises a salt of at least one aminotriazine compound selected fromthe group consisting of melamine and a condensate thereof with at leastone member selected from the group consisting of the sulfuric acid andan alkanesulfonic acid, and the flame-retardant auxiliary (B) comprisesan aromatic epoxy resin.
 18. A resin composition according to claim 1,wherein the base resin (R) comprises a mixture of a first resin and asecond resin, the first resin is a polybutylene terephthalate or apolypropylene terephthalate, the second resin is a polyethyleneterephthalate, the proportion of the first resin relative to the secondresin [the first resin/the second resin] is 30/70 to 80/20 in a weightratio.
 19. A resin composition according to claim 16 or 17, wherein theflame retardant (A) is 10 to 120 parts by weight and the flame-retardantauxiliary (B) is 0.001 to 5 parts by weight, relative to 100 parts byweight of the base resin (R).
 20. A resin composition according to claim16, wherein the proportion of the flame retardant (A) relative to thearomatic resin (B1) is 99.99/0.01 to 20/80 in a weight ratio.
 21. Aresin composition according to claim 1, wherein the base resin (R)comprises at least an aromatic polyester-series resin, the flameretardant (A) comprises a salt of at least one amino group-containingtriazine compound selected from the group consisting of melamine and acondensate thereof with at least one member selected from the groupconsisting of the sulfuric acid and the sulfonic acid, and theflame-retardant auxiliary (B) comprises at least one member selectedfrom the group consisting of acetyleneurea, uric acid, a salt of amelamine or a condensate thereof with cyanuric acid, and melamine or acondensate thereof, wherein, in the flame retardant (A) and theflame-retardant auxiliary (B), the melamine condensate is at least onemember selected from the group consisting of melam, melem and melon. 22.A resin composition according to claim 1, which further comprises atleast one component selected from the group consisting of anantioxidant, a stabilizer, a dripping inhibitor, a lubricant, aplasticizer and a filler.
 23. A resin composition according to claim 1,which further comprises an antioxidant in a proportion of 0.01 to 3parts by weight relative to 100 parts by weight of the base resin (R).24. A resin composition according to claim 1, which further comprises astabilizer in a proportion of 0.01 to 10 parts by weight relative to 100parts by weight of the base resin (R).
 25. A resin composition accordingto claim 16, which further comprises a dripping inhibitor in aproportion of 0.01 to 5 parts by weight relative to 100 parts by weightof the base resin (R).
 26. A resin composition according to claim 16which further comprises a lubricant in a proportion of 0.01 to 2 partsby weight relative to 100 parts by weight of the base resin (R).
 27. Aresin composition according to claim 1 or 16, which further comprises aplasticizer in a proportion of 0.01 to 20 parts by weight relative to100 parts by weight of the base resin (R).
 28. A resin compositionaccording to claim 1 or 16, which further comprises a filler in aproportion of 0.1 to 100 parts by weight relative to 100 parts by weightof the base resin (R).
 29. A process for producing a flame-retardantresin composition, which comprises mixing (R) a base resin, (A) a flameretardant recited in claim 1, and (B) a flame-retardant auxiliaryrecited in claim
 1. 30. A shaped article formed from a flame-retardantresin composition recited in claim
 1. 31. A shaped article according toclaim 30, which has, as an electrical property, a comparative trackingindex of not less than 300 V, and has, as a flame retardancy, aflame-retardant performance of V-2, V-1 or V-0 in a flame retardancytest measured by using a test piece having a thickness of 0.8 mm inaccordance with UL94.
 32. A shaped article according to claim 30, whichhas, as an electrical property a comparative tracking index of not lessthan 350 V, and has, as a flame retardancy, a flame-retardantperformance of V-0 in a flame retardancy test measured by using a testpiece having a thickness of 0.8 mm in accordance with UL94.
 33. A shapedarticle according to claim 30, which is an electric or electronic devicepart, an office automation device part, an automotive part, or amechanical part or machine element.
 34. A shaped article according toclaim 30, which is a connector part, a switch part, a relay part, atransformer part, a breaker part, an electromagnetic switch device part,a focus case part, a capacitor part, a motor part, a copying machinepart, or a printer part.
 35. A process for producing a shaped article,which comprises injection-molding a flame-retardant resin compositioncontaining (R) a base resin, (A) a flame retardant recited in claim 1and (B) a flame-retardant auxiliary recited in claim 1.